Mechanical Metamaterials and Their Engineering Applications

REVIEW
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Mechanical Metamaterials and Their

Engineering Applications
James Utama Surjadi, Libo Gao, Huifeng Du, Xiang Li, Xiang Xiong,
Nicholas Xuanlai Fang,* and Yang Lu*
1. Introduction
In the past decade, mechanical metamaterials have garnered increasing
Mechanical properties of materials have
attention owing to its novel design principles which combine the concept of
been one of the most fundamental and
hierarchical architecture with material size effects at micro/nanoscale. This widely studied areas in materials, owing to
strategy is demonstrated to exhibit superior mechanical performance that its crucial importance for real-life applica-
allows us to colonize unexplored regions in the material property space, tions. For centuries, the development of
including ultrahigh strength-to-density ratios, extraordinary resilience, and materials has solely relied on the modifi-
cations of its composition to alter mechan-
energy absorption capabilities with brittle constituents. In the recent years,
ical properties. Despite being effective, it
metamaterials with unprecedented mechanical behaviors such as negative usually takes more than a decade for a
Poisson’s ratio, twisting under uniaxial forces, and negative thermal expan- newly discovered material to be in the
sion are also realized. This paves a new pathway for a wide variety of market. Over the course of history, the
multifunctional applications, for example, in energy storage, biomedical, range of accessible materials kept on
acoustics, photonics, and thermal management. Herein, the fundamental growing, allowing us to select a more
suitable material for specific applica-
scientific theories behind this class of novel metamaterials, along with their
tions.[1–3] However, there are often definite
fabrication techniques and potential engineering applications beyond mechan- couplings between the intrinsic properties
ics are reviewed. Explored examples include the recent progresses for both of these materials, such as the intimate
mechanical and functional applications. Finally, the current challenges and coupling between strength and density,
future developments in this emerging field is discussed as well. where high strength materials are generally
high in density and vice versa.
On the other hand, numerous materials
found in nature often exhibit intriguing
properties unachievable with conventional
materials.[4,5] These natural materials, particularly cellular
materials, have evolved over the course of several million years
such that they developed an optimized architecture which could
span over multiple hierarchies across different length scales.[4–11]
Prof. Y. Lu, J. U. Surjadi, Dr. L. Gao
Department of Mechanical Engineering
For instance, the highly complex porous architecture of a bone core
City University of Hong Kong consisting of intricately-shaped ligaments and density gradients
Kowloon, Hong Kong SAR, P. R. China [email protected] allows it to achieve a much higher structural efficiency compared to
Prof. N. X. Fang, H. F. Du, Prof. X. Xiong most of the synthetic cellular materials developed by humans,
Department of Mechanical Engineering which possess significantly less sophisticated architectures and
Massachusetts Institute of Technology are far from ideal.[10,11] Another well-known example on the
Cambridge, MA, USA
E-mail: [email protected]
exploitation of architecture is the comparison between the Great
Pyramid of Giza and the Eiffel Tower. The Eiffel Tower is
Prof. Y. Lu, J. U. Surjadi, Dr. L. Gao, Dr. X. Li
Nano-Manufacturing Laboratory (NML) approximately twice as tall as the Great Pyramid of Giza but
Shenzhen Research Institute of City University of Hong Kong exhibits similar structural integrity and is almost three orders of
Shenzhen 518057, P. R. China magnitude lighter due to its hierarchical and three-dimensional
Prof. X. Xiong architecture.
National Laboratory of Solid State Microstructures and School of Although the concept of incorporating architecture into
Physics materials may not seem new,[12] the recent developments
Collaborative Innovation Center of Advanced Microstructures
Nanjing University in advanced manufacturing technologies such as additive
Nanjing 210093, China manufacturing (AM), also known as 3D printing, has enabled
the fabrication of cellular materials with complex architectures
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/adem.201800864. across several length scales, with feature sizes down to the
nanometer scale for a wide range of materials.[13–17] This brings
DOI: 10.1002/adem.201800864
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about another benefit to the mechanical properties of materials,

typically known as the “size-effect”, exhibited in certain James Utama Surjadi received his
nanomaterials where decreasing the size of a material down B.E. degree in Mechatronic
to the nanoscale allows them to exhibit unusual properties, such Engineering from City University of
as increase in strength compared to its bulk counterpart, also Hong Kong (CityU) with first class
known as the “smaller is stronger” trend in materials.[18–26] honors in 2017. He is a recipient of
Altering the topology of mechanical metamaterials such that it the Hong Kong PhD Fellowship
exhibits unique and tailorable properties (e.g., tunable stiffness, Scheme (HKPFS) and is currently
negative Poisson’s ratio, negative compressibility, vanishing pursuing a PhD in the Department
shear modulus) arising from rationally engineered deformation of Mechanical Engineering at CityU
mechanisms is possible as well. Along with the improvement in under the guidance of Prof. Yang Lu.
computational methods developed over the years, mechanical
metamaterials, which utilize the synergy between topology, Nicholas X. Fang is currently a
material composition and in some cases, “size-effect” in professor of Mechanical Engineering
nanomaterials, have the potential to produce novel materials at MIT. He also serves as chief
with unprecedented properties that approaches the theoretical scientist of BMF Material
limits of materials and could be optimized for specific industrial Technologies, a technical startup
applications across multiple disciplines. Figure 1 exhibit spunoff from his research group of
examples of previously reported mechanical metamaterials 3D micronanomanufacturing and
across multiple length scales, with unit cell and feature sizes nanophotonics at MIT. He received
ranging from a few millimeters to a few hundred nanometers. his BS and MS in physics from
In this review, the core principles behind mechanical Nanjing University, and his PhD in
metamaterials will be initially discussed. The section will serve mechanical engineering from University of California Los
as a brief introduction to the main classes of mechanical Angeles. Professor Fang’s areas of research look at
metamaterials and highlight the benefits that arise when unique nanophotonics and nanofabrication.
structural design principles and nanomechanical size-effect are
combined to exhibit unprecedented properties, deformation Yang Lu is currently an Associate
behaviors, and multifunctionalities that could not be achieved in Professor in the Department of
conventional materials. Subsequently, upon understanding Mechanical Engineering at City
the classification and related terminologies in the field, the University of Hong Kong (CityU). He
numerous fabrication methods that have been employed to directs the Nanomanufacturing
synthesize metamaterials across various length scales will Laboratory at CityU Shenzhen
be discussed, including their main principles, benefits and Research Institute, which focuses on
limitations. Finally, several notable examples of mechanical micro/nanoscale 3D printing and
metamaterial for both mechanical and functional applications mechanical metamaterials. He
will be discussed in greater detail, followed by a perspective on obtained his BS degree from
the possible future developments in the field with regards to Nanjing University and PhD degree from Rice University.
metamaterial design and modeling, fabrication, testing and Before joining CityU, he did postdoctoral research in MIT
characterization methods, and application potentials beyond for about two years.
traditional mechanics. This will mainly be used to introduce
works that have contributed to the significant advances in the
field and could serve as the foundation for future major
developments. The authors’ outlook in the field will provide new honeycomb. Evolution through billions of years has given them
researchers in this emerging field with possible directions which the internal structures which provide structural privileges as well
could be further investigated upon and hopefully lead to the as other beneficial properties. In many cases, the primary
industrial application of mechanical metamaterials across function of such cellular materials is to enhance the mechanical
multiple disciplines. properties, such as cancellous bone which gives a stiff support in
a weight-efficient way by incorporating pores and cavities.[11,29]
In recent years, these cellular structures have been adopted as
2. Utilizing Architecture, Size Effect, and tools in the design of mechanical metamaterial to manipulate
the structure-property relationship, resulting in the emergence
Mechanism
of novel metamaterials with unprecedented properties.
2.1. Structure of Cellular Materials Using architectural features to elicit desired functionality
will shift the material creation paradigm from structure driving
Cellular materials are basically consisted of intersecting (an processing and material properties to the desired material
interconnected network of) struts and plates which form the property driving the architecture and fabrication method.
edges and faces of the unit cells, and these small compartments Feasibility of this “reverse” material construction approach is
are packed and assembled together to fill the space.[27,28] Cellular gated by the ability to understand and predict mechanical
solids are widely found in nature: cork, wood, coral, sponge, and response of these metamaterials, or materials whose properties
Figure 1. Examples of 3D architected cellular materials with unit cell sizes spanning across multiple orders of magnitude in length scale, from tens of
millimeters to several hundred nanometers. a) A transformable origami-inspired metmaterial actuated by pressurizing its unit cells.[65] b) Hollow Ni–P
microlattice synthesized by Self-Propagating Polymer Waveguides (SPPW), electroless plating, and polymer etching.[127] c) A hierarchical microlattice
consisting of octet unit cells fabricated via Large-Area Projection Micro-Stereolithography (LAPμSL).[36] d) Tetrakaidekahedron microlattice printed using
Projection Micro-Stereolithography (PμSL).[34] e) A pentamode metamaterial with ultra-large bulk modulus to shear modulus ratio fabricated using Two-
Photon Lithography (TPL).[187] f) Hollow alumina nanolattices synthesized by TPL, atomic layer deposition and oxygen plasma etching.[16] g) High
entropy alloy coated nanolattice fabricated via TPL and subsequent magnetron sputtering.[149] h) Glassy carbon nanolattices made by TPL, followed by
pyrolysis.[14]
are controlled by their engineered structure rather than by Lattice materials, which will be discussed further in the later
atomic composition alone, where a new design parameter, sections, are commonly referred to as a sub-category of open-cell
feature size, plays a critical role. The research in the field of cellular materials which are composed of a large number of well-
architected metamaterials has profound implications not only defined architected structural elements, such as slender beams
for understanding the fundamental physics of the unique or rods, and could be generated by patterning its characteristic
effects that emerge in nano-materials, but also for proliferating unit-cell periodically in space. For a lattice to be considered and
these so-called size effects into the design of real materials. This act as a material, the number of unit-cells must be sufficiently
approach could fundamentally shift the way people think about large such that the length scale of the loading applied is longer
the creation of materials, with the concept of the reverse design than its lattice elements; otherwise, it would behave as a
of materials shifting the paradigm of material creation away structure instead of a material. The incorporation of a lattice
from relying on classical processing routes, which are structure could have a significant impact in expanding the
notorious for coupling properties like strength and density; material property space, especially at low densities.[1]
with strong materials also usually being very dense and heavy
and vice versa.
Therefore, understanding the mechanics of cellular materials 2.2. Bending versus Stretching-Dominated Architectures
is crucial to be able to exploit the benefits of architecture into
synthesizing metamaterials with tunable mechanical properties Bending-dominated structures, such as conventional foams,
at various length scales. In general, the mechanical properties of typically deform by bending of its interconnecting members
cellular materials can be defined by the material properties of its (such as struts and plates), whereas stretching-dominated
constituents, architecture, and relative density. Relative density cellular materials, which can be represented by a triangulated
is defined as the ratio of the cellular material density to the arrangement of such interconnecting members, deform through
density of a solid made of the same constituent material. Cellular the uniaxial compression or tension of its elements. Their
materials are either closed-cell or open-cell, and their deforma- topological configuration determines whether they are bending-
tion mechanism is usually categorized into two types, namely, or stretching-dominated. The dimensionless scaling law pro-
bending-dominated and stretching-dominated.[30,31] For an posed by Gibson and Ashby[1,21] for generic cellular materials
open-cell foam, its microstructures consist of a network of can semi-quantitatively describe the distinctive deformation
interconnected struts arranged in a three-dimensional (3D) mechanisms of closed-cell and open-cell foams, and within each
space. On the other hand, a closed-cell foam contains plate-like type of these foams each individual cell could either deform via
faces of a certain thickness and length. stretching or bending of its constitutive members depending on
the material distribution as well as cell topology. In the linear changes in the beam length are permitted and nonlinear out-of-
elasticity regime where microscopic strain does not exceed plane displacements of nodes could invalidate the linear
elastic limit of the constituent material, the effective Young’s equation assumption. Specifically, when all connection points
modulus of general strut-based structures can be expressed are similarly situated, the minimum connectivity of nodes for an
2
open-cell lattice to be stretching dominated is Z ¼ 6 for 2D
in terms of relative density: EEs ρρ , where E is the Young’s
s architectures and Z ¼ 12 for 3D case,[24] and a special type known
modulus of the cellular/architected material, Es is the Young’s as octet-truss has been observed to exhibit near-linear scaling
2
modulus of the constituent solid material, and ρρ represents in stiffness with relative density.[34] The connectivity refers to
s
the number of struts interconnected at a node.
the relative density of the cellular material with respect to the On the other hand, the infinitesimal deformation of plate-like
density of the constituent material. The scaling ratios with structures and closed-cell foams are governed by different
respect to relative density (ρ/ρs) for the effective Young’s mechanisms. Observing that the linear elastic deformation of
modulus (E/Es) and strength (σ/σy) of a bending- and stretching- these cellular materials is the sum of three contributions,
dominated architecture are shown in Figure 2a and b.[32] From namely, cell-wall bending, cell-face stretching and cell-face
this relationship, we can see that the strength gain of a bending, the cumulative effects can be derived in the following
stretching-dominated structure in comparison to a bending- scaling expression[35]:
dominated structure increases as the relative density of the
cellular material or lattice is decreased, and this could exceed a 2 2
E ρ ρ ρ
factor of 30 at a relative density below 0.1%.[30,33] ¼ C1 ð1 ϕÞ þ C2 ϕ2 þ C3 ð1 ϕÞ3
Es ρs ρs ρs
Maxwell conjectured a topological criterion relating numbers
of nodes and bars which determines whether stretching or
bending dominates in the deformation of the lattice structure. where Ci are the coefficients of proportionality, ϕ is the fraction
This was later argued to be a sufficient but not necessary of material distributed within cell edges as opposed to cell faces.
condition, with a few paradoxical exceptions if higher orders of The third term includes a quadratic relative density and becomes
Figure 2. Examples of bending- and stretching-dominated behavior in cellular materials. a), b) Influence of relatively density with the mechanical
properties of a bending- and stretching-dominated cellular architectures, respectively.[32] c) Stretching-dominated, rigid topology (Z ¼ 6) constructed
from rigid triangular unit cells.[102] d), e) Periodically-rigid, theoretically stretching-dominated topologies consisting of non-rigid unit cells, Z ¼ 5 and
Z ¼ 4.[102] f) Non-rigid, typically bending-dominated topology (Z ¼ 4) constructed from non-rigid unit cells.[102] g) Non-rigid topology which for the
indicated load case behaves fully stretching-dominated representing the least weight optimum. Unit cells are shaded in gray.[102]
insignificant compared with the leading first order for most hierarchy in these metamaterials allows for increased flexibility
closed-cell foams with low relative densities, thus rendering cell- to tune its mechanical properties.
face bending effects negligible. In this case the material
distribution between cell-edge and cell-face determines the
dominating deformation mechanism in plate-based or closed- 2.3. Origami/Kirigami-Inspired Metamaterials
cell structures.
While a stretching-dominated architecture is more beneficial In addition to the bending and stretching-dominated cellular
for structural applications due to its weight efficiency in materials described in the previous subsection, there are
handling external loads, a bending-dominated structure also other ways of altering the topological configuration of
accounts for lightweight and highly compliant materials. mechanical metamaterials such that it exhibits other novel
Alternately, it is also possible for us to make use of a multi- properties beyond those offered by bending and stretching-
scale or hierarchical structural configuration commonly found dominated architectures. Another class of mechanical meta-
in natural materials such as bone, bamboo, wood, and materials, primarily origami, and kirigami-inspired metamate-
nacre.[1,4,5,31] The structures in Figure 3 are examples of rials, have attracted increasing attention due to its ability to
hierarchical lattices in which a single strut is made up of an exhibit deformation mechanisms that would induce desirable
assembly of smaller lattices.[36] Increasing the structural mechanical properties, such as multistability, ultralarge
Figure 3. Multi-scale hierarchical lattice architectures that can be optimized for a specific application. Stretching-stretching configuration for highest
specific strength and stiffness. Bending-bending configuration for highest compliance. Bending-stretching and stretching-bending configurations for
intermediate cases.[36]
deformation, programmable stiffness, static morphing, and also occurs naturally in leaves and embryonic intestines.[61–63]
negative Poisson’s ratio.[37–42] Most of these mechanism-based They typically arise when thin sheets are restricted to a surface
metamaterials takes inspiration from the aesthetically pleasing and undergo biaxial compression. The 2D fold pattern forms a
patterns and design of origami (derived from the Japanese words lattice which can be characterized by two static crease lengths
“ori” and “kami”, meaning “to fold” and “paper’, respectively) or and one static plane angle. Each Miura-ori unit cell is
kirigami (from “kiru”, meaning “to cut”, and “kami”, meaning mechanically bistable, and by switching between states via a
“paper”)-inspired geometries. They are essentially based on reversible pop-through defect, the bulk properties of the overall
the plate-and-hinge mechanism, which are plates linked by tessellated structure could be reversibly tuned. Silverberg et al.
compliant hinges to form intricate geometries with tunable have created a metamaterial of the Miura-ori tessellation that has
deformation mechanisms, allowing for zero energy, free motion. tunable compressive modulus by varying the locations of the
The designability of such origami/kirigami-inspired metamate- pop-through defects.[39] Recently, Fang et al. have developed
rials allow them to potentially be used in a variety of applications, another method of achieving programmable stiffness in origami
such as in mechanical parts (e.g., pulleys, levers, gears, and metamaterials by proposing a nonflat-foldable single-collinear
linkages), electronic devices, medical stents, DNA nanofabrica- (SC) pattern.[41] The SC unit cell, which can be heterogeneously
tion, and the popular shape morphing materials.[43–50] constructed by two different flat-foldable Miura-ori unit cells,
Origami-inspired metamaterials, as their name implies, relies exhibited self-locking at a prescribed configuration, providing an
on the principles of folding and assembling typically planar or extra degree of freedom beyond the basic Miura-ori pattern.
2D materials into intricate 3D structures, although there are also Therefore, the SC unit cell has two different deformation modes:
many examples of origami metamaterials that have cellular pre-locking folding and post-locking pressing. Before the self-
architectures in 3D space, allowing for increased the degree of locking occurs, it deforms by the folding mode, exhibiting
freedom. The geometries of these type of mechanical materials relatively low stiffness due to the bending of the creases. In the
are generally based on two main parameters, namely, creases pressing mode after self-locking, the stiffness of the unit cell
and vertices, and its overall shape are governed by the quantity, increases significantly, which is attributed to the bending or
magnitude, sequence, and orientation of the folds.[51,52] For twisting of the facets.
instance, the creases refer to the locations of the localized folds The traditional square-twist pattern fundamentally has
on which the folding operations are made, whereas the creases with zero degrees of freedom and should not be
endpoints at which the creases intersect with another are called foldable. This is because the four-fold rotational symmetry of the
vertices. The regions bounded by the creases and vertices are structure dictates a cyclic set of geometric constraints on the
called faces. To determine how the creases are folded, a creases that define the central square facet. However, Silverberg
mountain-valley assignment is typically used. The mountain et al. have proposed a model which is foldable by utilizing the
creases refer to where the face on either side of the crease are plastic deformation induced by facet bending (Figure 5).[48,54,64]
rotated into the page, whereas the opposite occurs for valley Thus, the proposed square-twist model has two distinct
creases.[51,53,54] Alternately, it is also possible to determine the deformation modes: creasing and facet bending. The combina-
direction of the folds in terms of folding angles.[37] Positive tion of facet bending and the non-zero rest angle of the creases
folding angles forms valleys and the negative folding angles allow the structure to be plastically set when the patterned sheet
form mountain folds. Due to the restrictions imposed by the fold is folded, uncovering hidden degrees of freedom. A critical plane
network, origami metamaterials could exhibit highly nonlinear angle determines whether the square-twist pattern is mono-
deformations, with energetic landscapes arising from torsional stable or bistable. The inability to describe the deformation by
spring interactions as opposed to the central-force linear creasing alone, as with most of the other origami-inspired
springs.[37] metamaterials, drastically increases the complexity for its
Among the various origami patterns, the periodic Miura-ori computational modeling or simulation and is thus not widely
pattern is arguably the one which has attracted the most studied yet.[48] The non-periodic Ron Resch pattern (Figure 6)
attention and will thus be discussed in more detail in this was initially proposed by Resch in the 1960s and 70s, and its
section.[39,40,55–57] Its derivatives and other emerging patterns tessellation can be generated by the insertion of a star-like folded
which has garnered considerable interest in the recent years, tuck.[59,60] Lv et al. have studied the mechanical behaviors of
such as the square twist[54] and non-periodic Ron Resch several metamaterials derived from the Ron Resch patterns and
patterns,[58–60] will also be discussed briefly. Its unique have demonstrated its remarkable load bearing capability under
properties, such as negative Poisson’s ratio, and potential uniaxial compressive force.[58] The results also imply that
applications of such programmable metamaterials will be increasing the order of symmetry of the generalized Resch
discussed further in section 2.6 and 2.7. These representative patterns would increase its compressive strength even further.[60]
fold patterns have also inspired other derivatives which exhibit It is important to note that origami-inspired metamaterial
novel properties unattainable by the basic configuration. The designs are not only restricted to planar surfaces or arrangement of
Miura-ori tessellated folding pattern (Figure 4) is mathematically the patterns, but it can also be extended into 3D space.[43,44,65–74]
a herringbone pattern consisting of unit cells with four This implies that it is possible for us to design mechanical
coordinated ridges formed by convex mountain and concave metamaterials that combine the geometrical benefits of archi-
valley creases. As the four creases intersect, vertices are formed, tected cellular materials (e.g., high specific strength in micro/
binding equal-area parallelogram arranged with an inversion nanolattices) with origami-inspired design principles (e.g., those
symmetry.[39] This pattern was initially proposed to pack solar that could induce programmable stiffness, bistability, multi-
cells efficiently for space missions,[55] although the morphology stability). Thus far, two ways have been known to be able to
Figure 4. Miura-ori tessellation and its characteristics. a) Schematic illustration of the Miura-ori pattern in its folded state tessellated to form
herringbone-like pattern, showing n1 vertices in x1 direction, and n2 vertices in x2 direction.[58] b) Miura-ori tessellation in its planar or unfolded state,
where the shaded region represents a single unit cell and locations of mountain and valley creases.[58] c) 3D graphical representation of the Miura-ori
tessellation in its folded state, showing the vertex angle, e and static plane angle, α.[39] d) 3D reconstruction of a distorted Miura-ori tessellation with a
centrally located pop-through defect (PTD) highlighted in red, used to alter the compressive modulus of the overall metamaterial.[39] e), f) Optical
images of Miura-ori with crystallographic defects: e) edge dislocation and f) grain boundary arising from several adjacent edge dislocations.[39]
incorporate origami patterns into 3D space, which are stacking and could be done through periodic transformations of its 2D origami
interleaving. Schenk et al. stacked individual folded layers of the patterns, combining it into folded origami tubes, and tessellating it
Miura-ori pattern, and the resulting metamaterials exhibit not only in 3D space or into a desired lattice pattern.
high stiffness, but is also flat-foldable.[40] Fang et al. have also used Besides origami-inspired metamaterials, kirigami can also be
stacking on multiple Miura-ori sheets to create 3D cellular origami utilized to produce mechanism-based metamaterials through
metamaterial that exhibits static non-reciprocity through bist- the introduction of various cuts into thin sheets of material.
ability, achieving a static mechanical diode effect.[65] Interweaving Kirigami design principles have allowed the elastic properties of
Figure 5. Square-twist tessellation and its folding behavior. a) Schematic illustration of a square-twist tessellation in its unfolded state, where the shaded
region indicates a unit cell. The red lines on the unit cell represents the mountain creases and the valley creases in blue. The plane angle is represented by
ϕ, L is the characteristic length, and x is the Euclidean distance, which quantify macroscopic configuration between its folded and unfolded states.[64] b)
Folding process of the square-twist pattern.[48] c) Schematic of a self-folding polymer-gel trilayer square-twist unit, where folding is actuated by the
temperature dependent swelling of the hydrogel (pink) region.[64] d) Optical image of the fabricated polymer-gel square-twist unit.[64] e) Hysteretic
folding/unfolding of the self-folding trilayer square-twist unit as a function of temperature.[64]
Figure 6. Ron-Resch tessellation. a) Schematic illustration of an origamizer and Ron Resch pattern, both consist of surface polygons and hidden tucks.
However, the tuck in a Ron Resch pattern can be partially folded, whereas the vertex of the origamizer keeps the tuck closed owing to the crimp folds.[60]
b) Folding process of a regular triangular Ron Resch tessellation.[60] c) 3D Ron Resch tube via interweaving multiple partially folded Ron Resch pattern
into a tubular geometry. Uniaxial compression on the tube results in reduced diameter due to the negative Poisson’s ratio of the geometry (discussed in
Section 2.7), accompanied by drastically enhanced rigidity due to the fully folded state of the Ron Resch unit cells.[58]
materials to be altered drastically, achieving ultra-large strains or undergo brittle-to-ductile transition in its deformation mecha-
topological changes.[75–77] For instance, it has managed to nism.[92,93] For instance, it has been shown that at the nanoscale,
successfully transform one-atom-thick graphene sheets into the ductility of a generally brittle polymer photoresist can be
resilient and moveable structures.[78,79] Kirigami-patterned enhanced by 300% when the material is patterned into a
sheets also exhibit out-of-plane deformation or buckling, microlattice architecture. By utilizing polymer microlattice
providing a path to create complex 3D structures at various structures with strut diameters of less than 100 μm as templates
length scales for mechanical or functional applications.[45,80–85] for electroless deposition, it is possible to form metallic
Furthermore, besides using kirigami-patterned sheets as 2D microlattice structures where the truss member wall thickness
metamaterials or 3D structures via out-of-plane deformations, it is in the nanoscale regime.[94]
can be combined with origami design principles to create folded A size-dependent strengthening where the effective strength
structures with intricately patterned cut surfaces.[86,87] This of a material is enhanced significantly, several times compared to
hybrid approach expands the design space for mechanism-based its macroscale counterpart, could also be observed as the length-
metamaterials even further. scale of the material is decreased down to the nanoscale.[18–24]
This is because in real-life materials, the fabrication of a
bulk material would introduce numerous imperfections in
2.4. Size Effect in Micro/Nanoscale-Materials the material, such as grain boundaries, voids, cracks, and
dislocations, which results in the actual strength to be
The material size effects at the nanoscale show that as the considerably below the theoretical strength of the material.
external dimensions of materials are reduced to the nanoscale, Therefore, although the theoretical strength of a brittle ceramic
their mechanical behavior will have a significant change and or ductile metals has been calculated to be around 1/10 and 1/30
exhibit unique phenomenon. At this circumstance, some times of its elastic modulus, the typical bulk strength in practice
materials will become much stronger,[88,89] weaker,[90,91] or even is around 1/300 times the modulus.[95] Thus, strength is greatly
dependent on the characteristic intrinsic size of the material, prioritize on the manufacture and mechanical properties of
which can be typified by the length scale of its microstructural mechanical metamaterials.
components, such as the size and distribution of the pre-existing
flaws or nanoparticles impurities. For a ductile metal, the
increase in strength could be explained by Hall-Petch relation- 2.6. Characterizing the Mechanical Properties and Behaviors
ship, which describes the material strengthening of polycrystals
when its grain size is reduced.[25,26,96,97] For a brittle material, its Mechanical metamaterials offer new possibilities for enhancing
fracture strength could be approximated according to Griffith’s the mechanical behaviors and properties of materials while
law, where the strength is inversely proportional to the square- offering multifunctional properties across various disciplines
root of the critical crack size.[98] In bulk materials, the typical owing to its customizability in design, size, and material
grain or crack size is well above the nanoscale, resulting in low constituents. Therefore, it is of vital importance for us to be able
yield or fracture strength.[95] to understand and quantify the typical properties of mechanical
As such, a well-known strategy to decrease the intrinsic metamaterials in order to accurately alter its properties and
features of a material is to reduce its overall extrinsic deformation behaviors for specific applications. In this section,
dimensions. When the size of the material is decreased and the basic mechanical properties (i.e., strength and stiffness) and
approaches the nanoscale, the size of its intrinsic flaws deformation modes of mechanical metamaterials will be
eventually becomes closer to the length scale of its extrinsic investigated, particularly focusing on the benefits arising
feature. In other words, as the size of a material gets smaller, through the incorporation of architecture and size effects.
the size of its defects or the probability of finding a defect also Employable characterization techniques for various length-
becomes smaller, and smaller defects leads to increased scales will also be discussed.
strength in comparison to its bulk values. This is often known Although the effects of size-effects on the strength of the
as the “smaller is stronger” phenomenon.[18,88,99,100] While material could be estimated by Griffith’s law or Hall-Petch
different materials follow different scaling laws, it is possible relation as discussed earlier, the wide range of materials available
that when the overall size of the material is reduced below a which results in contrasting behaviors between each type, the
certain critical value, which is usually in the order of 1–100 nm, absence of a universal scaling law, and defects or uncertainties
its effective strength could reach theoretical values. This has induced by different fabrication methods makes it difficult to
been observed several times in some crystalline metallic and quantify and predict accurately the size-effects in a lattice
ceramic materials.[18,101] It is this phenomenon which allows material. On the other hand, the effect of architecture on the
lattice materials with strut diameter or wall thickness in the strength of cellular materials could be applied at any length-scale
nanoscale to exhibit superior properties and novel mechanisms and is more easily predicted.[1,30,31,33] In general, the effective
which significantly exceeds that of macroscale lattice materi- strength, which represents the fracture strength of a brittle
als.[14–16,102,103] However, this is not always the case, and the material or the yield stress in a ductile material, and stiffness of
opposite, where the conventional “smaller is weaker” phenom- any cellular or lattice material can be predicted according to the
enon occurs, is also a possible outcome, such as the case with first-order scaling law.[30] Based on this law, the strength or
the hollow-beam nickel and gold lattices.[34,104,105] stiffness is a product of the strength of its constituent material,
relative density which is raised to a constant value depending on
the topological configuration of the cellular or lattice material,
2.5. Computational Methods and Topological Optimization that is, stretching- or bending-dominated, and a geometric
constant which indicates the degree of anisotropy of the
The computational method is commonly used to design and structural unit. Increasing the anisotropy of the lattice
investigate the mechanical properties of the mechanical architecture such that all its elements are perfectly aligned with
metamaterials. With the help of the computational method, the direction of loading will result in the maximum value of the
one can have a comprehensively understanding its properties. geometric constant, thus maximizing the effective strength in
Some experiments could be too costly or time consuming to be the loading direction.[102,105,122,123] In a cellular material,
performed multiple times. Thus, computational mechanics can especially nanolattices where the dimension of its elements is
be used to give a set of system parameters which results in at the nanoscale, size-effect could significantly affect the
optimal performance, such the type and geometric configuration mechanical properties of its constituent material. In addition,
which would give the highest strength at the lowest possible at very low relative densities, the cell wall (2D) or struts in the
density possible among different structures. lattices (3D) can be slender enough such that it will experience
Topological optimization is an important method to obtained beam buckling and collapse before the reaching the failure
structures with desirable mechanical properties. Phase field strength of the material. In this case, the strength of the
method,[106] topological derivative,[107] level-set methods,[108–112] constituent material would be substituted by the buckling
bubble method,[113] evolutionary procedures,[114] and density- strength, which can be determined in accordance with Euler
based methods[115] are topology optimization methods which buckling criterion.[31,124] For hollow lattices, where the strut is
have undergone great development. Numerous researchers have shell element instead of a solid beam, the material will
also given their review on the topology optimization meth- experience shell buckling instead of beam buckling.[13,36,125]
ods.[116–120] Xia et al. have especially given a comprehensive Therefore, the governing deformation or failure mechanism of
review about the structural optimization on advanced structures the lattice metamaterial, whether its material fracture or
and materials recently.[121] Therefore, in this paper, we would buckling, is determined by the overall dimensions of its
elements and the critical values can be found using the equations In addition to lattice materials, reversible and/or programmable
proposed by Meza et al. and verified experimentally.[15,16,126] buckling can also be induced in origami and kirigami meta-
Although buckling will generally reduce the effective materials by pressure and folding,[65,69] thermal heating,[134,135]
strengths of conventional materials, it is the core mechanism mechanical straining,[45,136] humidity/water,[137] electric field,[138]
which enables deformability in a lattice material. As buckling is magnetic field,[139] or irradiation,[80,140] depending on its constitu-
an elastic phenomenon and that due to this, the intrinsic stresses ent materials.[141] Buckling or facet bending is generally
in the buckled beam has yet to reach its fracture or yield strength, responsible for the unique deformation behaviors, recoverability
the lattice has the potential to recover after external loading.[103] and mechanical properties exhibited by origami or kirigami
This has been observed in a hollow ceramic micro- and metamaterials due to its bistable unit cells. By controlling the
nanolattice that are made of both brittle and ductile materials. deformation behaviors (e.g., through origami/kirigami design
Examples of this are the alumina nanolattices demonstrated by principles or other topological configurations), it is possible to
Meza et al. and the nickel microlattice developed by HRL, which balance the deformability and strength in mechanical metama-
are shown in Figure 7.[16,127] It is important to note that while it terials to cater specific applications.[67–69,142–144] Fang et al. have
could recover, the post-yield strength and Young’s modulus of shown that different deformation modes (i.e., contraction,
the structure decreases compared to its un-deformed counter- shearing, bending, and facet bending) could also be achieved in
part due to the formation of localized fractures at several places. a generic 4-degree vertex origami sheets and blocks by reducing
However, the structures typically exhibit stable cyclic behavior geometric constraints.[38] As the types of deformation behaviors
subsequently.[15,16,127–130] This mechanism is also responsible and mechanical properties arising from the bistability or multi-
for the layer-by-layer deformation in a lot of lattice materials, stability of various pattern geometries, orientations, and arrange-
which allows controlled dissipation of energy.[15,16,122,131–133] ments are too numerous to be discussed in this section, more
Figure 7. Examples of notable mechanical metamaterials. a) Hollow metallic microlattice demonstrating its ultralow density and excellent
recoverability.[127] b) Strong, lightweight, and recoverable hollow nanolattice out of brittle constituent (ceramic) fabricated after compression at 50%
strain.[16] c) Brittle fracture in hollow ceramic nanolattice with thicker walls, that is, larger thickness to strut diameter ratio, demonstrating the size-effect
in nano-scale ceramics.[16]
specific examples will be discussed in section 4. Stacked cellular enhanced flexibility in designing materials by controlling its
origami consisting of tubular channels could exhibit increasing deformation or failure mechanism, occasionally through the aid
stiffness by pressurizing it as well. Pressurizing the channels of an external stimuli. Incorporating structural hierarchy into the
would result in a fold that maximizes the enclosed volume, thus design will also allow us to enhance a particular property of the
any deformations that result in reduced volume would be resisted mechanical metamaterial, such as recoverability, due to a more
by pressure.[69,73,145] localized deformation or failure.[1,15,36,75]
Testing and characterizing the mechanical properties of
metamaterials are typically done using standard testing methods
for traditional materials at the bulk scale. For instance, a macro- 2.7. Unique Properties and Multifunctionalities
scale material testing system is usually used to investigate the
compressive, tensile, and bending behaviors of mechanical In recent years, the increasing interest in mechanical meta-
metamaterials at the millimeter or centimeter scale and up to materials has brought upon the novel incorporation of
large-scale meter-sized samples.[58,146,147] Due to the unique interesting concepts which adds new functionalities, drastically
behaviors often exhibited in metamaterials, in-situ mechanical broadening its application potential. These include negative
testing is generally preferred. This involves the inclusion of an Poisson’s ratio (auxetics), negative compressibility, negative
optical camera (or high-speed camera for high strain rates) to thermal expansion, and vanishing shear modulus. In this
observe the deformation of such materials. Optical microscopy, section, the unique properties of mechanical metamaterials due
Scanning Electron Microscopy (SEM), or even Helium Ion to distinct topological configurations will be briefly discussed,
Microscopy (HIM) could be employed to observe the post- along with its potential applications. These properties also
mortem morphologies upon failure during testing.[147,148] SEM enable mechanical metamaterials to be applied beyond
and HIM could also be used to observe the deformation modes mechanical applications. Related examples of mechanical
of metamaterials at the micro or sub-micron scale, occasionally metamaterials in various fields will be discussed in section 4,
with sample feature sizes down to tens of nanometers (e.g., while this section will focus on the basic principles behind each
nanolattices).[14,16] Various types of in-situ micro-tester and unique property.
quantitative nanomechanical testing platforms (e.g., nano- and Poisson’s ratio v is defined as v ¼ eeTL , where, eL and eT are the
pico-indenters) are inserted into the sample chamber for strains in the loading direction and the direction transverse to
mechanical testing of micro-scale samples.[14–16,122,149] Owing the loading direction. The original definition of the Poisson’s
to the intricate 3D geometries achievable by a variety of ratio is based on the homogeneous continuum where
fabrication methods, full geometrical characterization of deformations are uniform within the material. However, due
mechanical metamaterials could not be accomplished easily to the localized deformations around hinges and nodes,
by only surface-deep characterization tools. Focused Ion Beam mechanical metamaterials could be designed to exhibit a
(FIB), which utilize a finely focused beam of ions (typically negative effective Poisson’s ratio (auxetics), which is counter-
gallium) and high beam currents to cut micro/nano-sized intuitive behavior under external loading.[165] The overall
materials, could be coupled with SEM to observe the 3D response of auxetics is thus different from the local behavior
microstructure of a mechanical metamaterial through serial of its constituents.[43] In other words, they expand under tension
sectioning, but often results in the destruction of the and contract under compression. Materials with negative
specimen.[150,151] Therefore, several imaging techniques could Poisson’s ratio have attracted increasing attention after Lakes
be employed to visualize the 3D morphologies. Optical confocal manufactured the isotropic foams with negative Poisson’s
microscopy, which utilizes pinhole optics with a laser probe, is a ratio.[166] A re-entrant structure was used to explain the
powerful tool to obtain 3D imaging of optically transparent mechanism of the foams with negative Poisson’s ratio. During
mechanical metamaterials with sub-micron resolution based on the past several decades, design and fabric structures with
the reconstruction of 2D micrographs at different depths.[152–155] negative Poisson’s ratio have been an important part of the study
X-ray tomography is a technique frequently employed to of materials with negative Poisson’s ratio.[167–174] Re-entrant
characterize 3D microstructures as well and provides an structures, rotation of rigid/half rigid joints, and chiral
additional capability of being able to probe optically opaque structures are typical structures with negative Poisson’s
samples. This involves using finely focused X-rays to examine ratio.[172,175–177] Origami-inspired metamaterials (e.g., Miura-
the specimen and an X-ray camera is used to capture the ori planar sheets or stacked cellular solid) are also known to
transmission radiograph.[156–160] Although X-ray tomography is exhibit negative Poisson’s ratio in both its 2D and 3D
typically used to observe micro-scale structures, non-destructive tessellations.[38,40] The definition of the Poisson’s ratio is no
nano-scale X-ray imaging have also been used recently to observe longer limited to bulk materials and could be extended to suit for
nano-scale specimens. Alternately, electron tomography via the materials with various topologies and hierarchical micro-
Transmission Electron Microscopy (TEM) could be used to structures. The unique deformation behaviors of auxetic
characterize 3D structures at nanometer-scale resolution by metamaterials, most of which mainly relies on the folding
passing through a fine beam of electrons at incremental degrees and unfolding of its non-rigid elements, allows them to possess
of rotation about the center of the sample.[161–164] However, many desirable mechanical properties such as tunable stiffness,
achieving the appropriate sample thickness for TEM, which is high energy absorption, superior fracture, indentation and shear
generally at sub-micron scale, could be destructive. resistance, variable permeability, etc. This provides new
In summary, the combination of size effect and topological opportunities in the design of non-rigid mechanical metama-
configuration (e.g., lattices, origami, kirigami) provides us with terials with applications in but not limited to shape morphing
materials, flexible actuators, sensors, medical prostheses, Compressibility is a term used to quantify the relative volume
dampers or shock absorbers, and textiles.[41,43,178–182] Auxetic change of a solid or fluid in response to applied pressure or
lattices based on a three-dimensional re-entrant honeycomb pressure variation and could be expressed as the inverse of bulk
design shown in Figure 8 allows the alteration of the Poisson’s modulus, K.[189–191] Therefore, compressibility is typically a
ratio of the material, from negative to zero and even to positive positive value, which means that a material will deform along the
values, only by making slight modifications in the geometry of its direction of the external force, in exception of a very limited
unit cell structure.[43,183–186] number crystals, such as lanthanum niobite,[192] cesium
Another intriguing and new type of mechanical metamate- dihydrogen phosphate,[193] zinc dicyanoaurate,[194] isomorphous
rials is the pentamode metamaterials, commonly known as Se and Te phases,[195] as well as an orthorhombic high-pressure
metafluids and an example is shown in Figure 9.[32,43,187,188] paratellurite (TeO2) phase,[196] which have been shown to display
These metamaterials possess very high bulk modulus in negative linear compressibilities (- dL/LdP). In other words, the
comparison to its shear modulus, which is close to zero. The material will expand under tension or contract under compres-
high bulk modulus results in minimal volumetric changes in the sion, regardless of its response in the traverse directions.
material during deformation, which indicates a Poisson’s ratio Negative responses based on open/cellular materials or activated
close to 0.5. Pentamode metamaterials also have very small shear through dynamic excitation have previously been observed.[197]
modulus and this allows the material to almost “flow away” For instance, porous solids under hydrostatic pressure (P)
under shearing force, akin to a fluid. The combination of these conventionally contract in all directions, meaning that its linear,
two concepts in pentamode design means that it is hard to area (- dA/AdP), and volume (- dV/VdP) compressibilities are all
compress yet easy to deform the metamaterial by shear positive values. However, sorption or infiltration of the medium
deformation. However, the complicated three-dimensional particles could cause the porous solid to expand, which
structures were unable to be fabricated prior to the recent corresponds to a negative compressibility.[198–201] Certain
advances in additive manufacturing techniques; not to mention composites have also been shown to exhibit negative elastic
the point-point connections are almost impossible to achieve. Its constants in response to acoustic waves at certain resonant
mechanism and properties will be further discussed in a later frequencies or a decreasing response force as the applied
section with respect to more specific examples. Pentamode deformation increases.[202–204] Although it is possible to obtain
metamaterials or lattices have been demonstrated to be able to be negative compressibilities in those systems, negative compress-
applied in elastomechanical cloaking by allowing a material to be ibility for a closed system (which refers to the inherent material
rendered “unfeelable”.[188] property) is deemed to be impossible for a natural material as it is
Figure 8. 2D and 3D auxetic metamaterials. a–c) 3D lattices with tailorable Poisson’s ratio from a) positive, b) to approximately zero, c) to negative.[183]
d) 2D instability-based auxetic structure which undergoes a reversible buckling-like instability under compression.[43,184] e) Schematic illustration of the
main principle behind auxetics.[43]
Figure 9. Pentamode metamaterials which have a significantly higher bulk modulus than shear modulus. a) Schematic illustration of the main principle
behind pentamodes.[71] b), c) Example of a polymeric pentamode lattice fabricated by direct laser writing,[37,82] d), e) A core-shell “unfeelability” cloak
based on pentamode metamaterials which could be used to elastically hide mechanical objects along its lines.[83]
thermodynamically unfavorable.[205] However, Nicolaou pro- Other potential applications of mechanical metamaterials
posed the concept of negative compressibility transition to which makes use of its topological flexibility, size effects, and
design mechanical metamaterials with negative compressibil- material constituents includes the creation of architected
ities.[189] The unique condition is met as a force causes the thermal heat exchangers and insulators,[212–218] photonic crystals
system to move from a stable state to another metastable state. with unique optical properties,[80,219–223] phononic crystals with
This concept is analogous to bistability, commonly observed tailorable bandgaps for acoustic cloaking,[224–227] battery electro-
in origami/kirigami-inspired metamaterials, where energy is des with optimized topology for electron transport, electrochem-
stored or supplied to a deformed element, such as post-buckled ical and mechanical properties,[228–232] and bio-scaffolds or meta-
tubes. Qu et al. have also designed and experimentally verify a biomaterials, which involves the rational design of an optimized
3D micro-structured metamaterial consisting of hollow crosses combination of mechanical, mass transport and biological
with negative static volume compressibility.[206] Materials with properties to enhance tissue regeneration.[233–239] Recently,
negative responses could potentially be used for a range of microlattices for tunable electromagnetic shielding has also
important applications, including artificial muscles, actuators, been reported.[240]
pressure sensors, and MEMS/NEMS.[189,197,207]
Recent progresses in mechanical metamaterials have led to
the discovery of 3D elastic chiral metamaterial that responds to 3. Fabrication Methods: Advantages and
compression with a twisting motion (Figure 10),[208] program-
Challenges
mable stiffness by utilizing bistable unit cells and self-locking
upon mechanical loading,[39,41,57] and those that exhibits static There are various fabrication techniques that could be employed to
non-reciprocity showing significantly different output displace- synthesize mechanical metamaterials, most of which involves a
ments under excitation from different sides, as well as one-way type of additive manufacturing method, with a few exceptions.
displacement amplification.[65,209] The fabrication of lightweight While some new methods such as self-assembly could also be used
multi-material structures with tunable negative thermal expan- to fabricate these architected cellular or lattice materials and are of
sion, in which a structure contracts in one or more direction interest due to its potential benefits in manufacturing metama-
upon heating and is analogous to negative compressibility, has terials in a large scale, they are still in the premature stage. A well-
also been demonstrated.[210,211] controlled topology is difficult to achieve, which means that it will
Figure 10. Chiral mechanical metamaterials that exhibits a twisting motion upon uniaxial mechanical loading. a) Unit-cell design. b), c) Finite element
simulation on the unit-cell and overall metamaterial. d) Chiral metamaterial fabricated by direct laser writing with different topological configurations to
investigate its effect on the amount of “twisting” produced.[208]
be difficult to accurately simulate its behaviors and properties. through extrusion of a nozzle. This could be done through a variety
Furthermore, the diversity of structures that could be fabricated is of ways, ranging from melting a solid filament, to depositing
still very limited currently. Therefore, the techniques discussed in droplets of ink onto the substrate which is usually flat. Among this
this section will mainly involve the various kinds of additive category, Fused Deposition Modeling (FDM) and Direct Ink
manufacturing techniques that have been proven to be able to Writing (DIW) are typically well-known to be able to produce fairly
successfully fabricate these metamaterials, while other proven but intricate structures for a wide variety of base materials. FDM
less well-known or potential methods will be mentioned briefly. involves heating of a solid filament, typically made of a
Common post-processing techniques employed after the fabrica- thermoplastic material such as Polylactic Acid (PLA) and
tion of the architected structures to enhance the properties of the Acrylonitrile Butadiene Styrene (ABS), up to the point of melting
material will also be mentioned. In this section, we will categorize and extruding it out onto a flatbed through a heated nozzle. The
and evaluate the types of additive manufacturing techniques that melted filament rapidly cools down below its glass transition
have been developed thus far into 3 main classes, namely, 3D temperature and solidifies again upon contact with the ambient air.
printing through ink-based, photo-solidification, and powder- However, the rapid cooling would often induce shrinkage of the
based methods. Although each class does not directly represent a material deposited, due to thermal expansion during deposition,
specific technique, there is a generalized concept for each type. causing the printed structure to be warped or poor adhesion on the
Emphasis will be put on recent techniques which have been known bed surface.[241] A heated bed is usually used when 3D printing
to yield novel results and properties in the field of mechanical materials that have high coefficient of thermal expansion. The
metamaterials, with potential to be applied industrially for a melted filament is subsequently deposited layer-by-layer until the
multitude of applications. Subsequently, alternative proven 3D structure is fabricated, where the shape printed at each layer is
techniques on manufacturing mechanical metamaterials besides represented by the 2D cross-section of the designed structure.[242]
3D printing will be discussed, some of which could be coupled with A schematic illustration of the FDM 3D printing setup is shown in
3D printing for enhanced efficiency and/or scalability. Figure 11a. For 3D cellular structures, a support material deposited
through a secondary nozzle is typically needed for successful
fabrication. This method is used to fabricate partially or fully solid
3.1. 3D Printing through Ink Extrusion and Jetting structures with minimum feature sizes of approximately few
hundred micrometers.[31,243] Figure 11b and c are representative
One of the most commonly-used 3D printing methods of cellular structures fabricated using FDM.[148,243] While it is mainly
fabricating architected cellular materials or mechanical metama- used for 3D printing thermoplastics, the filaments could be filled
terials, especially at the meso- and macro-scale, involves the direct with other particles/fibers, such as carbon black, carbon fiber,
deposition of the material constituent onto a substrate or bed wood, metallic powders, ceramic powders, etc. to enhance the
Figure 11. Extrusion-based 3D printing methods. a) Schematic illustration of the basic working principle and setup for Fused Deposition Modeling
(FDM). b) A polymer octet-truss lattice fabricated by FDM.[243] c) A composite lattice with polymer core and Ni outer shell synthesized through FDM and
electroless plating.[148] d) Schematic of the working principle behind Direct Ink Writing (DIW) using viscoelastic inks. e) 3D microlattice fabricated by
multi-material DIW.[118] f) Balsa wood-inspired fiber-filled epoxy honeycomb composite printed using DIW.[252]
functionality or mechanical properties of the printed part.[244] The techniques such as sintering or curing is typically required to
important factors to consider for FDM 3D printing which will produce stiff structures and improve structural integrity.[242]
affect the print quality are the mechanical and thermal properties DIW allows for a wide range of materials to be 3D printed,
of the filled or unfilled thermoplastic filament used, such as the similar to or exceeding that of the capabilities of FDM-based
consistency in filament diameter, porosity, density, moisture printing when combined with various post-processing techni-
content, glass transition temperature, as well as the melt flow ques.[137,228,231,249–251] Particularly, the wide array of inks with
characteristics of the melted filament.[241,242,245] diverse properties developed by Lewis et al., such as epoxy filled
Another good alternative to FDM is DIW, where a viscoelastic inks[252] and silicone-based elastomeric inks,[253] had major role
or viscoplastic ink in a syringe is extruded through a nozzle onto in the success of this method over the past decade.
the printing bed surface under an external force such as Understanding the rheological properties of the inks used is
pressurized gas, mechanical piston, or screws.[246] This typically crucial for DIW. Generally, the inks used for DIW can be
done under ambient conditions, although the ink and bed could characterized through the Herschel–Bulkley model, where they
be heated or cooled to a desired temperature using a heating or have shear yield stress and shear thinning behavior. Thus, as the
cooling compartment.[247] DIW could sometimes be performed applied pressure is increased, the ink is extruded more readily
with the nozzle immersed under a gel-like solution as through the nozzle but adopts high shear yield stress as they exit
well.[228,248] A schematic illustration of the 3D printing process the nozzle which gives the inks a solid-like response. The
is shown in Figure 11d. This method has been used to effectively properties of these yield-stress inks could easily be tuned by
produce mechanical metamaterials of varying porosities, from a changing the ratio of its constituent materials. The values of
solid beam or strut to randomly porous architectures. Akin to viscosity for these inks typically lie in the range of 102–106 MPa s,
FDM-based additive manufacturing, infusing the ink with other which is dependent on the desired shear rate. DIW has been
particles such as ceramic particles allow the fabrication of a wide demonstrated to be able to produce high quality prints with an
variety of structures using different materials. However, as it extensive range in terms of the minimum feature size printable,
uses a viscoelastic ink to print, the resulting structures produced ranging from 1 micrometer to a few hundred micro-
are usually soft in nature.[242,246] Therefore, post-processing meters.[242,246] Figure 11e and f exhibit examples of cellular
structures synthesized using DIW.[118,252] In the recent years, producing finer features in comparison to ink-based or powder-
this method has also been of extensive interest in the fabrication based techniques as it is not restricted by the physical dimensions
of biocompatible or functional hydrogels and aerogels. For of the nozzle or powder used, respectively. However, some of the
instance, Tan et al. has developed a biocompatible composite ink new advances in 3D printing technologies have significantly
based on poly(vinyl) alcohol (PVA) and Pythagel to print 3D increased the range of feature sizes that can be printed for ink-
scaffolds which aims to mimic soft organic tissues.[247] Zhu et al. based or powder-based methods to rival that of light-based printing
has fabricated a hierarchical graphene aerogel supercapacitor by techniques.[242,256,257]
combining DIW with other post-processing methods such as Light-based 3D printing techniques mainly involve the
supercritical drying which exhibits excellent electrochemical fabrication of 3D structures using either a UV light or laser
performance, significantly surpassing that of bulk graphene source directed into a photopolymer resin. Stereolithography
aerogels.[227] (SLA),[259,260] one of the most used 3D printing technique used
In addition to FDM and DIW, ink-based 3D printing methods today, is the first method of 3D printing available which typically
could also include several types of inkjet-like 3D printing which uses a UV light to cure a photosensitive resin layer upon layer by
involves direct jetting of droplets onto a flat or powder bed such pointwise polymerization and has been responsible for the
as Polyjet printing, Binder jetting, and hot-melt printing.[254,255] successful fabrication of several novel microlattices.[131,261,262]
Unlike DIW, these methods typically employ low-viscosity fluids. Although SLA[259,260] are perhaps the most well-known,
For instance, hot-melt printing uses wax-based inks that are emerging techniques such as Two-Photon Lithography (TPL)
melted during droplet formation and solidifies upon impact.[242] (also known as Direct Laser Writing),[14,16,263] Projection Micro-
Polyjet printing is a combination of both ink-based and light- Stereolithography (PμSL),[34,264] Self-Propagating Photopolymer
based 3D printing (which will be discussed further in the next Waveguide (SPPW),[127,265,266] Continuous Liquid Interface
section), in which it uses a photo-sensitive polymer droplet that Production (CLIP),[267] are responsible for most of the recent
polymerizes upon exposure to an ultraviolet (UV) source. Binder successes in the utilization of light-based 3D printing techniques
jetting involves depositing droplets of a binder solution onto a for the fabrication of mechanical metamaterials. As such, these
powder bed to fuse the powders together in the desired position methods will be the primary focus of this section.
layer-by-layer, eventually forming the 3D solid part or struc- TPL (Figure 12a) makes use of a highly-focused femtosecond
ture.[32] Other novel methods developed recently that involves pulsed laser beam with a wavelength of typically 780 nm to cure a
microdroplet deposition includes the Aerosol Jet technology,[256] photopolymer resin in a multiphoton absorption process. As this
FluidFM technology,[257] Laser Induced Forward Transfer is a non-linear second-order process which is several orders of
(LIFT),[258] which have been proven to be able to fabricate 3D magnitude weaker than single photon absorption, the intensities
cellular structures through the use of nanoparticle inks, ion of light required to polymerize the photosensitive resin is much
solutions, and molten metal, respectively. For all these ink-based higher than linear absorption. Thus, a pulsed laser source is
3D printing methods, the successful fabrication of a structure used to provide high intensity pulses. To sculpt a 3D structure
depends on the quality of drop formation, which is based on using such method requires the photoinitiator present in
several factors on both the ink properties and printing the monomer be transparent to light with the laser source
parameters. This includes the ink’s viscosity, density, surface wavelength such that single photon absorption is inhibited but
tension, droplet diameter, velocity at which the ink is ejected, and absorbs light at half wavelength which takes twice as much
diameter of nozzle used. These parameters must be controlled energy as compared to full wavelength. Therefore, if there is an
precisely such that either the viscous forces do not dominate area where at least two photons with a wavelength equal to the
which will cause the ink to get clogged in the nozzle or the single wavelength of the laser source are absorbed simulta-
inertial forces of the ink to dominate, causing the ejected ink to neously, the total sum of energies produced in that area will be
splash onto the bed surface.[241,242] sufficiently high to induce polymerization.[263] The regions at
which these two photons meet and possess energy higher than
the threshold value for polymerization is also known as a voxel
3.2. 3D Printing through Photopolymerization and is typically elliptical in shape.[268] These small focused
regions could be moved in 3D space by altering the laser focus,
Due to the boom of 3D printing in the past decade, there has been allowing the fabrication of 3D structures without any support,
an increasing number of 3D printing methods available which are provided that the 3D structures could support themselves during
able to synthesize high quality architected cellular materials in a the polymerization process. Otherwise, additional support may
wide range of sizes. The success of mechanical metamaterials be required. This method could typically achieve writing speeds
such as nano/microlattices in the recent years has mostly been in the order of mm s1 with the minimum printable feature size
attributed to its ability to not only utilize the architecture, but also in the range of several hundred nanometers.[103] TPL is currently
the size effect in materials which allows for unconventional the 3D printing technique which has been proven to be able to
properties to be discovered. Among the techniques available thus fabricate highly complex architectures with the finest details,
far, light-based 3D printing, which utilizes the concept photo- achieving resolution of down to 100 nm with more complex
polymerization to create solid structures, is the most used method configurations.[268,269] Although the working area is usually in
to synthesize intricately designed micro- or nano-architectures the range of only a few hundred micrometers, larger structures
with ultrafine features, especially in the order of few hundred in the millimeter or centimeter scale could be achieved by
nanometers to several micrometers.[13,14,16,36] This is because stitching multiple writing fields.[270] Although TPL is commonly
light-based 3D printing methods are generally capable of known to be able to only fabricate polymeric structures, several
Figure 12. Schematic of the various AM processes involving photo-solidification with images of their representative samples. a) Two-Photon lithography
(TPL), or otherwise also known as Direct Laser Writing (DLW).[14] b) Large-Area Projection Micro-Stereolithography (LAPμSL).[36] c) Self-Propagating
Polymer Waveguides (SPPW).[265,266] d) Continuous Liquid Interface Projection (CLIP).[267]
post-processing techniques such as Physical Vapor Deposition detailed summary of these works along with other notable
(CVD),[105,150,271] Chemical Vapor Deposition (CVD),[229] Atomic reports will be explained in a later section.
Layer Deposition (ALD),[15,16,272] and Electroless Plat- The working principle of PμSL is almost analogous to Digital
ing[122,127,273,274] can be used to produce high quality metallic Light Processing (DLP) 3D printers such that it uses a UV light
and ceramic nano/micro-architectures through sacrificial tem- source to project a 2D pattern and polymerize a photosensitive
plating. Recently, Vyatskikh et al. have also synthesized a dense resin layer-by-layer to form the 3D structure.[264,275] In each layer
metallic nanolattice by altering the photosensitive resin defined by the 2D cross-sections of the sliced 3D model, an array
formulation, producing a pre-metallic polymer resin.[17] A more of UV light-emitting diodes (LEDs) is used to project an entire
layer onto the liquid photopolymer resin through a dynamic which is dependent on the length of the propagated waveguide,
digital mask, inducing polymerization of the photosensitive could range from about 100 mm to above 25 mm. Generally, the
resin in the shape of the projected image. Subsequently, the maximum achievable material thickness is approximately 100
polymerized layer is lowered down further into the photopoly- times the strut diameter of the lattice unit cell. However, larger
mer bath by a certain distance determined by the slicing height, thicknesses could also be fabricated by exposing the photopoly-
allowing for a new layer of the resin to be cured on top of mer to the 2D mask at different heights, which results in
the previous layer. This process is continuously repeated until multiple layers akin to that of layer-by-layer fabrication in
it forms the 3D structure. Generally, the thickness of the conventional 3D printing methods. SPPW has been shown to be
polymerized layer lies between 10 and 100 mm, which is able to fabricate lattices out of stiff,[265,266,285,286] viscoelastic,[287]
dependent on the depth of penetration by the UV light source. and pre-ceramic polymers.[288] One main advantage of SPPW
This in turn is determined through the combined effect of the compared to other 3D printing methods is the ability to fabricate
curing characteristics of the photosensitive resin used and 3D structures at a substantially higher rate (>1 m2 min1 for
several key process parameters, such as power of UV source, continuous process) and scalability (fabrication area 0.4 m2).
exposure time, and concentration of photoinitiator in the CLIP is essentially an extended or upgraded version of DLP
monomer resin.[275–277] An extended version of PμSL which printers, such that it makes use of a transparent and oxygen-
aims to address the concerns regarding its scalability has been permeable window to be able to print parts continuously,
developed, and is known as Large Area PμSL (LAPμSL).[36,278] It ultimately removing the need for a sequential layer-by-layer
integrates a reconfigurable SLM with a galvanometric mirror process.[267] This results in the fabrication of smooth parts,
scanning system to produce architectures in a scanning-like absent of any model slicing artifacts. The main distinctive
pattern, in which the area of projection could be moved laterally feature of CLIP in comparison to DLP and other light-based 3D
and the projected image changes depending on the respective printers is the existence of an oxygen-inhibited dead zone.
location of the layer pattern. A schematic illustration of the 3D Oxygen-inhibition is traditionally thought of as a problem, often
printing setup is shown in Figure 12b.[36] One of the main leading to incomplete curing and surface tackiness in most 3D
advantages of LAPμSL over TPL despite the lower resolution is printers that perform photopolymerization in the air. However,
its scalability, meaning that it can produce larger structures has CLIP utilizes an oxygen-permeable window between the UV
been shown to be able to produce macroscale cellular source and photosensitive resin which controls the concentra-
architectures in the order of tens of centimeters, as opposed tion of oxygen within a thin layer between the window and cured
to below 10 cm in TPL. Akin to other light-based 3D printing resin. This thin layer is typically in the order of tens of
techniques, although the primary type of material used are micrometers and is also known as the “dead zone”. The “dead
polymers (either stiff and elastic),[279] other types of materials zone” enables the continuous supply of liquid uncured resin
such as ceramics could also be printed by a pre-ceramic polymer between the advancing part being printed and the oxygen-
resin,[262,280,281] Multi-material PμSL has also been developed permeable window, consequently allowing a structure to be
which could be used for shape-morphing architectures, continuously drawn-out of the photopolymer bath. A schematic
sometimes known as 4D printing.[282] illustration of the CLIP process and setup is shown in
While SPPW (Figure 12c)[265,266] is comparable to other light- Figure 12d. CLIP has been able to produce structures with
based 3D printing techniques such as SLA,[260] DLP,[283,284] minimum feature sizes (such as strut diameter) of approxi-
CLIP,[267] and PμSL/LAPμSL[36,264] in a sense that it uses UV mately 50 mm using a wide variety of material resins, primarily
light to cure a photopolymer resin, it is a unique technique which polymers which includes rigid and flexible polyurethanes,
utilizes an angled exposure to polymerize the monomer. SPPW silicones, epoxies, etc. One of the most important features that
allows the fabrication of intricate lattice structures by a single 2D need to be controlled in CLIP is the thickness of the “dead zone”
exposure plane instead of the stacked layer-by-layer approach. layer, which significantly affects the capabilities of the 3D printer,
This is done by using a collimated UV beam which is passed such as speed and resolution. There are a number of crucial
through a 2D mask containing a series of patterned circular material and processing parameters that need to be considered
apertures passing it into the liquid photomonomer bath. As the when using CLIP, such as the photon flux that indicates
photomonomer is exposed to the collimated UV light, self- the number of incident photons per unit area per unit time,
propagating photopolymer waveguides will form originating absorption coefficient of the photoinitiator/resin which is
from the aperture. This polymerizes the photosensitive determined by the product of wavelength-dependent absorptivity
monomer bath in both the direction of the collimated beams and photoinitiator/resin concentration, and resin curing dosage
and at the points of intersections, resulting in an interconnected which quantifies the reactivity of the photosensitive resin at a
3D array of polymer struts. Upon removing the uncured certain monomer-photoinitiator combination. Some of the main
photopolymer solution, an open-cell 3D architecture or micro- advantages of CLIP include remarkably high printing speeds
lattice could be obtained. The topological configuration of each (500 mm h1), meaning that a 3D structure of about 5 cm could
lattice unit cell can be controlled by changing the pattern and be fabricated in under 10 min, and more isotropic parts due to
diameter of the circular apertures in the 2D mask, spacings the absence of layer-by-layer morphology.
between the apertures, as well as the orientation and incident Another notable recent method which aims to tackle the
angle of the collimated UV beams. SPPW could be used to create speed-associated concerns regarding 3D printing and has
lattice structures in the micro-scale, with typical minimum achieved promising results is the Volumetric AM (VAM)
feature size such as strut diameter of about 10 mm. In each UV technique.[289] VAM could fabricate complex millimeter scale
beam exposure, the overall lattice material thickness created, 3D polymeric geometries in the span of a few seconds without
any supporting structures. This was done through the powder as the starting material. Recently, there is also another 3D
superposition of patterned optical fields from multiple beams printing method, Diode-Based AM (DiAM), that aims to solve one
which are subsequently projected into a photopolymer bath. of the most inhibiting problems faced by powder fusion
This is similar to Multi-Beam Interference Lithography techniques, which is the speed of fabrication, allowing for
(MBIL),[93,290,291] except that it projects entire 2D images in significantly increased printing speeds through the fusion of an
the 3 principal directions. entire layer simultaneously instead of point-by-point.
SLM is arguably the most commonly used commercial 3D
printing method for manufacturing metallic structures or
3.3. 3D Printing through Powder Fusion components thus far and has been used to fabricate mechanical
metamaterials mainly for structural applications and biological
3D printing techniques that make use of powder fusion typically implants/prosthetics. The working principle of SLM is fairly
involves using a laser source to fuse powder particles together similar to SLS and DMLS and that it uses a fiber laser beam as
either through sintering or melting. Alternately, the powder may the energy source to fuse the powder at certain locations within
be fused by the aid of a binding agent, such as the case for binder the powder bed layer-by-layer through a raster-like movement. In
jetting explained earlier. Another type of pioneering 3D printing each layer, the printing process begins by melting the powder in
method in addition to SLA is the Selective Laser Sintering (SLS), the outer boundaries first, followed by melting of the powder
which is a combination of both light-based and powder-based 3D within the contour to form the dense part or strut. The recoating
printing technique that utilizes a laser source to sinter or fuse process between each layer is akin to SLS/DMLS. The printing
polymeric powders in a heated powder bed by a raster-like process is typically conducted in an inert gas filled chamber
pattern layer upon layer.[292,293] After each 2D layer, a new layer of to reduce the concentration of oxygen and hydrogen in the
powder is spread across the powder bed by a roller for resupply environment, preventing or minimizes the risk of oxidation and
before sintering another layer on top of the previously fused hydrogen pick up, respectively. The schematic illustration of the
layer. Once the 3D structure has been fabricated, it is removed SLM system is exhibited in Figure 13a.[241,304] The main
from the powder bed and might undergo further heat treatment difference between SLS/DMLS in comparison to SLM is that
in a furnace. A certain amount of the unused powder can usually for SLM, the powder is fully melted before being fused to form a
be recycled. One of the most important factors that affect the fully homogeneous part as it creates a melt pool which allows the
print quality is the shape, size, and distribution of the powder material used to consolidate prior to reforming and hardening,
used. Smaller powder sizes mean that the minimum layer but not for SLS/DMLS. In SLS/DMLS, the powder is simply
thickness would be lower, thus increasing its resolution and the heated to the point that it can be fused or merged together on a
minimum printable feature size of the cellular architecture. On molecular level and this temperature is lower than that of the
the other hand, the shape and morphology of individual powders melting point in most cases. Therefore, SLM typically produces
(e.g., roundness) affect the flowability and packing of the powder higher quality structures than SLS/DMLS, owing to the reduced
particles. Poor flowability, generally caused by high interparticle number of voids resulting in a denser part with superior
frictional forces, in a powder-based 3D printing could cause mechanical properties. However, SLS/DMLS can sometimes be
uneven distribution of the powder, resulting in inconsistent preferred over SLM, such as when 3D printing metals with
fusion of the powder and low packing density. The packing particularly high melting point such as tungsten or alloys with its
density of the powder bed can also affect the quality and elemental constituents having significantly different melting
consistency of the 3D printed structure considerably in terms of temperatures. In SLM, the varying melting temperatures might
the overall or bulk density of the produced part. In addition, the cause the process to be unstable. Akin to SLM, EBM involves
absorptivity of the powder used for a laser of a specific fully melting of the powder material as well, but uses a focused
wavelength is also an important parameter that needs to be electron beam from an electron gun instead of a laser source.
evaluated, which is crucial in determining the laser intensity Furthermore, as electrons are used to provide the energy to melt
required to fuse the powder particles together and produce a the powder, the printing process must be conducted in a vacuum
well-consolidated and dense 3D printed structure.[240,294] environment to reduce contamination to both the source and
In most powder-based 3D printing techniques, there are material. In contrast to SLM, EBM makes use of electromagnetic
generally four main categories of parameters that needs to be taken coils and lenses to deflect and focus the electron beam ejected by
into account to achieve high quality parts and structures, namely, the gun instead of optical lenses (Figure 13c).[241,304] The
the properties of the powder bed such as the material used and operating power and chamber temperature for EBM are usually
powder density, the laser and scanning parameters such as laser higher than in SLM and SLS/DMLS. The primary advantage of
power, wavelength and scanning speed, recoating parameters, and EBM compared to SLM is that it reduces the residual thermal
build environment. Direct Metal Laser Sintering (DMLS) is stresses within the part printed, resulting in reduced support
another technique which is almost analogous to SLS as it is based structures needed to obtain the desired shape. However, the
on the same principle, differing only in the technical parame- surface finishing is typically inferior to that of SLM (Figure 13b,
ters.[295–297] SLS is usually used when polymeric, ceramic, or glass d).[305,306]
powders are used, whereas DMLS is used when printing metallic SLS, DMLS, EBM, and SLM are sometimes classified as
or alloy structures. Other 3D common printing methods that Powder Bed Fusion (PBF), as they utilize a pre-deposited layer of
involves the use of powder fusion are Selective Laser Melting powder. PBF has been used widely to produce micro-architected
(SLM),[298,299] Electron Beam Melting (EBM),[300–302] and Directed lattices in many macro-scale applications such as in aerospace
Energy Deposition (DED),[303] although DED is not restricted to and biomedical implants. DED, which can occasionally be
Figure 13. Schematic illustration of the setup for AM processes involving powder fusion with images if their representative samples. a) Selective Laser
Melting (SLM). b) Example of a pentamode metamaterial fabricated by SLM.[306] c) Electron Beam Melting (EBM). d) Example of lattices printed using
EBM.[306]
interchangeable with Laser Engineered Net Shaping (LENS), mechanism, properties, and procedures. It is necessary to note
Laser Cladding (LC), Direct Metal Deposition (DM), and Laser that some of these methods have principles that can be similar to
Metal Deposition (LMD) is conceptually similar with PBF 3D or combined with additive manufacturing techniques to produce
printing techniques, especially SLM and EBM, in which it mechanical metamaterials.
involves a high energy thermal beam, typically a laser, to melt a Self-assembly is an effective and popular tool for the synthesis
metal on a flat substrate that eventually solidifies to form the 3D of either 2D or 3D materials at the micro/nano-scale. Thus, this
structure. However, the energy beam is focused on a continuous approach has been particularly useful for photonic and phononic
stream of powder or wire which is deposited directly onto the applications. This involves the bottom-up autonomous arrange-
substrate.[240,303,307] While both PBF and DED suffers from slow ment of components or building blocks into a specific
printing rates, researchers from Lawrence Livermore National structure.[309] While there are numerous materials that have
Laboratory (LLNL) have developed a novel method to solve this been studied for this process, it is outside the scope of this
problem by using an optically-addressable light valve (OALV), review. Thus, this section will only mention the successful and
which consists of polarization-selective nematic liquid crystal most relevant class of materials that could be self-assembled into
sandwiched between a photoconductor and transparent conduc- controllable 3D architectures, which is the main interest for this
tor, as a photo-mask to print an entire layer of metal powder at review. Colloidal crystals and block copolymers (BCP) are two of
once.[308] High power laser diode arrays are used to multiplex an the main families of material that could be self-assembled and
optical sheet and switched laser pulses are used to selectively are of increasing interest for the fabrication of mechanical
melt each powder layer. metamaterials. Assemblies of colloidal crystals could be formed
via a solution infused with micro- or nano-scale particles and
employment of slow evaporation times or other techniques (e.g.,
3.4. Alternative Methods electrophoresis).[310] The primary driving force for this method is
the secondary van der Waals interactions between the particles
As mentioned earlier, although additive manufacturing techni- and could be made using a wide range of material compositions,
ques have been the most popular choice for fabricating such as organic polymers,[311] bioparticles,[312] metals,[313,314] and
mechanical metamaterials, there are other fabrication methods ceramics.[315] High quality crystals up to the centimeter scale
which could be used, although they might be highly restricted could be produced, such as the fabricated nickel inverse opals
or less conventional. However, there are those that possess that covered areas greater than 1 cm2.[316] Colloidal crystal arrays
inherent advantages over certain additive manufacturing have been used as photonic,[311,312,315,317–319] acoustic,[320–322]
techniques for producing some type of metamaterials. There- and energy dissipative structures.[323] Furthermore, using
fore, this section will briefly describe their fundamental particles with various sizes,[324,325] modified substrates,[326] or
functionalized particles,[327–329] it is possible to create a wide strength which approaches theoretical limits, to resilient
range of crystal structures. BCP consists of two or more ceramics that does not fracture catastrophically upon mechanical
immiscible polymer blocks that are covalently joined end-to-end loading. In this section, several well-known reports on
resulting from microphase separation of its constituents.[330–333] metamaterials which focus on its unprecedented mechanical
The nano/micro-domains of each block depending on the properties and behaviors, such as mechanical resilience in
molecular weight and overall composition of the copolymers. ceramic structures, tunable stiffness, and negative Poisson’s
Numerous 2D architectures of BCP have been synthesized, and ratio, in the past few years will be investigated in more detail.
via confining BCPs in bounded regions, templating, or The hollow microlattices shown in Figure 7a and 14 fabricated
sequential processing of 2D BCP patterns into stacks, akin to using SPPW were developed by HRL Laboratories with its overall
3D-printing, 3D microstructures (e.g., helices, double gyroids) dimensions in the order of centimeters or larger. The densities of
could be formed.[334] While self-assembly possesses immense these microlattices can be as low as ρ ¼ 0.9 g cm3, which places
potential for the scaling up nano/micro-features onto bulk it into the ultra-light weight regime.[127] Materials in this ultra-
samples, the controllable geometries that could be formed are light regime are scarce, such as silica aerogels, carbon nanotube
still highly limited. aerogels, metallic, and polymer foams. Most of these have
Conventional laser cutting or high power pulsed laser ablation, random cellular architectures, resulting in the significant
which involves the removal of a solid through irradiation by a laser reduction of some certain properties (e.g., stiffness, strength,
beam, has been used to fabricate 2D auxetic re-entrant honeycomb energy absorption) compared to its bulk counterpart due to the
structures from polymers, as well as flat-foldable kirigami, and inefficient load transfer between its ligaments. For instance, the
origami metamaterials.[38,50,53,335–337] Similarly, Focused Ion stiffness or Young’s modulus (E) of stochastic materials scales
Beam (FIB) can also be used to create intricate 2D patterns at poorly with density in the ultra-light regime, generally following
the micro or nano-scale.[80] Ravirala et al. have also proposed E ρ3 as opposed to the conventional E ρ2 relationship
interlocking assembly, in which geometrically matched male- observed in unordered open-cell foams with higher densities.
female interlock combinations in adjacent particles are joined However, via the incorporation of architecture and structural
together to form an array or assembly. The assembly of interlocked hierarchy across various length scales, these microlattices exhibit
hexagonal plates deforms by particle translation and exhibit Young’s modulus that scales with density as E ρ2, along with
auxetic properties.[338] This method can be used as the base to impressive compressibility (98% recovery after uniaxial com-
fabricate interlocked 3D re-entrant honeycomb structures as pression at 50% strain). These properties make them desirable
well.[339] In addition to these techniques, interference lithography for acoustic, vibration, or shock energy absorption. The
(either multi-beam interference or phase mask interference) could microlattices are composed of hollow metallic struts with
also be employed to fabricate mechanical metamaterials.[340–343] In diameters on the order of 100–500 um and lengths of 1–4 mm;
principle, interference lithography is similar to the photopolyme- the wall thickness of the hollow cylindrical struts is on the order
rization-based 3D-printing methods described earlier. Interfer- of 100–500 nm.[127] SPPW is initially used to fabricate polymeric
ence lithography (IL) refers to the formation of 1D, 2D, or 3D scaffolds with a desired architecture.[265,345] In the subsequent
structures through the change in chemical functionality, (de) fabrication steps, the polymer scaffold is coated with a thin solid
crosslinking, or (de)polymerization of a (positive)negative-tone film, such as nickel phosphorus (Ni–P) using electroless
photoresist. This is caused by the emergence of a non-uniform deposition technique. The polymer is then removed through
intensity field as two or more light sources with different chemical etching via aqueous NaOH, leaving behind a fully
intensities, directions, phases, or polarizations, interfere with one hollow structure composed of the deposited material.[127,275] The
another.[290] It is also worth noting that a combination of these microlattice has a unique structural behavior that emerges as the
techniques, along with 3D-printing could be employed. For ratio between strut wall thickness, t, and strut diameter, D, falls
instance, the purposeful introduction of defects via TPL in 3D below a critical threshold of (t/D). This critical ratio is described
patterned structures created by DIW, IL, or self-assembly could be as (t/D) critical f (σY,s, Es, θ, emax), where θ is the lattice angle, σY,
done to increase its structural hierarchy for various pur- s, and Es are the yield stress and strength of the constituent
poses.[155,344] In addition, stimulus-responsive fabrication techni- material and emax is the maximum compressive strain on the
ques, sometimes referred to as 4D-printing, has also garnered microlattice.[274,346] As the ratio of the wall thickness of the struts
increasing attention in recent years. This utilizes the effect of to strut diameter falls below a critical value of (t/D) < 0.005 for
external stimuli (e.g., thermal heating,[134,135] irradiation,[80,140] the Ni microlattices, the lattice completely recovers after strains
pre-straining,[45,136] magnetic fields,[139] moisture/waster-induced greater than 50% of the lattice height.[345] The hollow nodes
swelling[137] etc.) in combination with the methods described in accommodate substantial bending moments, which occur at
this section to fabricate 3D architectures from 2D precursors. lower forces than would be required for Euler buckling of the
hollow struts, and this is the mechanism responsible for the
impressive recovery of the microlattice.[127,274]
4. Typical Examples of Mechanical Similarly-scaled micro-architectures have also been created
Metamaterials using PμSL.[34] In contrast to the bending-dominated micro-
lattices by HRL, this technique is capable of producing a variety
4.1. Mechanical Metamaterials for Structural Applications of different geometries, including the octet-truss, which has
sufficient nodal connectivity to be a stretching-dominated
Mechanical metamaterials have been known to exhibit uncon- structure.[1,274] Similar to the coating and etching process of
ventional mechanical properties, ranging from ultrahigh the HRL microlattices, the PμSL-produced microlattices can also
Figure 14. Design, processing, and cellular architecture of ultralight microlattices.[127] a) Polymer microlattice templates are fabricated from a three-
dimensional array of self-propagating photopolymer waveguides. b) The open-cellular templates are electroless plated with a conformal Ni–P thin film
followed by etch removal of the template. c) Optical image of the hollow Ni–P microlattice fabricated with this approach: 0.9 mg cm3. d) Images of two
as-fabricated microlattices along with a breakdown of the relevant architectural elements.
either be made entirely of monolithic polymer struts, or the highly compliant and are able to undergo large deformations prior to
polymer can serve as a sacrificial scaffold once they are coated failure. It contains structural features ranging from a few
with a material, such as Ni–P or alumina (Al2O3).[34] The polymer centimeters to the nanometer-scale with each order of hierarchy
can be removed either through chemical etching or pyrolysis. occupying an order in the length scale. One of the main benefits of
Under uniaxial compression, the behaviors of the hollow Ni–P or increasing the order of hierarchy in a material such as the
Al2O3 octet-truss microlattices agrees well with the scaling law microlattices in Figure 15 is the ability to decouple the certain
predicted by classical theory. These octet-truss structures inherent properties that would be impossible to achieve with a first-
outperform the HRL microlattices as predicted by classic order hierarchy. For example, as each strut of the 2nd order
cellular solids theory in terms of stiffness, which is attributed architecture is made up of its own 1st order lattice unit cells which is
to a change in characteristic deformation mechanism between also cellular, the length of the struts could be made much shorter for
bending- and stretching-dominated architectures.[34,124] a given relative density in comparison to a 1st order structure. The
Both types of these hollow microlattices have wall thicknesses in Euler buckling strength of a lattice structure discussed previously is
the size regime of where material size effects are observed, but the inversely proportional with the square length of its struts, thus
dimensions of their unit cells are too large to observe or capitalize shorter struts lead to increased buckling resistance.[36]
on the size effects. Therefore, their deformation behavior can be Nanolattices, fabricated by two-photon lithography, enable a
described from the structural point of view, which is independent of size reduction by three orders of magnitude from the micro-
material length scales. For example, if the microlattices were scaled lattices described above while still being amenable to the coating
up in a self-similar geometry, the mechanisms of deformations and scaffold removal steps. These architected materials have
would be consistent with those of the microlattices at smaller scales. dimensions down to the nanoscale, with typical strut lengths of
However, these microlattices still offer many novel properties that 3–20 mm, diameters of 150–500 nm, and wall thicknesses of
result from the interaction between structural features at various 5–600 nm.[13,16,105,271,272] Unlike the microlattices, the individual
length scales, such as their recovery and energy absorption building blocks that comprise nanolattices are small enough that
capabilities. For instance, the fractal-like hierarchical microlattice they cannot be resolved by the human eye. Their mechanical
produced by LAPμSL shown in Figure 15 exhibits increased properties depend on the combination of the size-dependent
buckling resistance in comparison to regular lattice structures, akin material properties and structural response and cannot be
to how the hierarchy in bone allows it to have extraordinary resilience predicted solely by scale-free continuum theories.[16,105,347]
to mechanical loading or how soft tissues such as skin could be Hollow gold nanolattices with octahedron geometry were
Figure 15. Example of a hierarchical polymer microlattice fabricated using Large Area Projection Micro-Stereolithography (LAPμSL).[36] a–c) Optical
images of the macro-scale lattice material consisting of hierarchical stretching-dominated octet unit cells. Scanning Electron Microscope (SEM) images
of the structural breakdown of a hierarchical octet unit cell which makes up the bulk lattice material. The scale bars in (c), (d), (f), (g), and (h) are 80 μm,
80 μm, 10 μm, 3 μm, and 2 μm, respectively.
fabricated via TPL, followed by sputtering, then polymer scaffold remained unchanged. This is contrary to classical mechanics of
removal through O2 plasma ashing. Their response to uniaxial cellular solids which predicts a constant strength and stiffness
compression as a function of lattice angle and wall thickness for all the nanolattice geometries explored in the study.[105] The
were investigated, and the results revealed that both geometrical interplay of structural and material size effects has also been
and material size effects could be exploited to elicit novel observed in structures with solid metal struts as the constituent
mechanical properties that would not exist in a larger version of a building blocks of the lattice and are created using a similar
self-similar structure alter the mechanical strength and stiffness method to the hollow nanolattices.[347] Similarly, Meza, et al. has
of a nanolattice material. By tuning the geometries of the lattices, successfully utilized atomic layer deposition to coat 5–60 nm
the strength and stiffness can be increased despite having thick Al2O3 onto the polymer scaffolds synthesized by TPL. The
constant deformation mechanism and relative density.[1,31,105] In polymer core was removed using a similar method as Au
their experimental tests, the relative density of the hollow Au nanolattices by plasma etching. Uniaxial compression experi-
nanolattices was kept constant at ρ ¼ 0.05 while the unit cell size ments of the octet-truss hollow nanolattices (Figure 7b, c) have
was varied from 5 to 20 mm, and strut wall thickness from 200 to demonstrated that through the optimization of wall-thickness to
661 nm.[105] The lattice angle of the octahedron unit cell, which is strut diameter ratio, it is possible to suppress brittle fracture in
defined as angle between the lattice hollow tubes and the nano-scale ceramics through elastic shell buckling as discussed
horizontal mid-plane of the unit cell, was increased from 30 to in Section 2. The optimized Al2O3 octet-truss hollow nanolattices
60 , for a fixed wall thickness of 300 nm. An increase of exhibited exceptional recoverability and could withstand up to
approximately one order of magnitude was observed in both the 80% strain.[16] Increasing the order of hierarchy of the hollow
strength and stiffness in these bending-dominated cellular nanolattices from a first order structure to a second order
solids. All the lattice samples, as revealed by experimental structure also increases recoverability of the ceramic nano-
observations and confirmed by analytical calculations, deforms lattices. The fractal hollow Al2O3 nanolattice fabricated by Meza
by the initial yielding and bending at the nodes which causes it to et al. shows unprecedented recoverability of up to 98% after
rotate, followed by bending of the hollow beams. To examine the being compressed to 50% strain.[15]
effect of material size effects on the 45 octahedron nanolattices, Bauer et al. has also demonstrated that the polymer
the wall thickness was varied from 200 to 635 nm and an nanolattice fabricated by TPL could be converted into glassy
increase of 150% in strength was observed while the modulus carbon through pyrolysis at 900 C.[14] During this process, the
lattice structure experiences a drastic volumetric reduction such pentamode metamaterials were fabricated.[350] Due to the large
that the size of the resulting carbon nanolattice is only 20% of the size of the sample, Schitttny et al. directly measured the static
initial polymer nanolattice, making it the smallest nanolattice shear modulus and the Young’s modulus. The ratio of bulk to
produced thus far. The glassy carbon nanolattice mainly consists shear modulus reaches as large as 1000. By combining analytical
of non-graphitic sp2-bonded carbon and its size allows it to coordinate transformations and numerical topology optimiza-
exhibit remarkable mechanical properties. It has a Young’s tion with latticed pentamode metamaterial design, Bückmann
modulus of 20–30 GPa, which makes it approximately 10 times et al. proposed a pentamode metamaterial-based elasto-mechan-
stiffer than that of conventional crosslinked epoxy resins such as ical cloak.[188] The three-dimensional polymer cloaking device
SU-8, and its specific compressive strength of up to 0.89 MPa with macroscopic size is fabricated by TPL process. The cloaking
kg m3 exceeds that of other microlattices by about six times. design was based on core-shell approach. The pentamode
Furthermore, the nano-honeycomb structure made of the same cloaking offers a solution to provide a rigid wall, whereas the
constituent material has been tested to achieve near theoretical surrounding as well as the shell exhibit small shear moduli. The
strengths under uniaxial compression. The ultrahigh specific pentamode lattice structures show very good mechanical
strength achieved leaves diamond as the only bulk material that cloaking performance under uniaxial compression force. This
has reached a notably higher strength to density ratio. This implies that it could be possible to elastically hide objects inside
ability to exploit the benefits from both architecture and size the metamaterial, making it “unfeelable”.
effects allows nanolattices to exhibit novel properties that have Origami/kirigami-inspired metamaterials provide a pathway
the potential to decouple the inherent strength-density relation- for tuning the deformation mechanism and properties of
ship between conventional material property theory. However, it mechanical metamaterials. Silverberg et al. developed a
is important to note that if these nanolattices were scaled up in a metamaterial using a tessellation of the flat-foldable Miura-ori
self-similar fashion, such that the smallest external dimension is pattern. Each unit cell is bistable, thus by switching the states of
increased above a few microns, the unique material properties certain unit cells via facet bending, the mechanical properties
present at the nano-scale would become less significant. Thus, it (e.g., stiffness) of the metamaterial could be rationally tuned. In
is still a challenge to sustain the nanoscale strength during scale their work, they demonstrated the switching via manual means,
up. Schematic illustrations of several known fabrication although other methods could potentially be used to switch the
processes to produce core-shell composites, hollow structures, states of unit cells or activate the pop-through defects, including
as well as glassy carbon nanolattices from polymer are shown in micromechanical actuators, robotics-based technologies, and
Figure 16a–c. Other strategies typically involve making alter- thermal actuation. These changing between states are also
ations to the initial polymer, such as the incorporation of reversible, demonstrating its potential in various applications,
ceramic/metal powders and solutions. such as deployable solar cells, self-folding robotic and polymer
Pentamode materials are a type of three dimensional systems.[39] Similarly, Silverberg et al. have utilized the
materials with unique elasticity. It has a single bulk modulus deformation of folded paper sheets caused by facet bending to
but zero shear rigidity. The elasticity tensor of pentamode uncover the hidden degrees of freedom in a square-twist pattern.
material can be written as C ¼ KII, in which I is a 2nd order They discovered that by varying the critical plane angle, it is
symmetric tensor, and K is the bulk modulus.[224,348] This form possible to achieve bistability through origami as the plane angle
of elastic moduli then is translated to a two dimensional 6 6 exceeds the critical value (25 ).[54] By fabricating a temperature-
matrix with single one non-zero eigenvalue. A face-centered- responsive polymer gel with the same folding pattern, the
cubic (fcc) “diamond-type” pentamode structure in which four metamaterial exhibits hysteretic folding dynamics as the
linkages meet at appoint was also suggested as a natural temperature was gradually increased and decreased.[54,351] This
candidate by Milton and Cherkaev. Although pentamode demonstrates its potential application as stimulus responsive
structure designs were proposed theoretically by Milton and and self-folding mechanical switches.
Cherkaev two decades ago, it have not been experimentally Besides planar tessellation of the origami-patterns, it is also
fabricated until 2012. Kadic utilized TPL to experimentally possible to arrange them in three dimensions by stacking or
realize the first double-cone pentamode metamaterial sam- interweaving. Fang et al. have utilized the stacking of multiple
ple.[187] The pentamode polymer metamaterial synthesized Miura-ori sheets to exhibit multistability in a dual-cell chain
contains 1024 units with a total volume of approximately 2 structure. They stacked unit cells consisting of two different
mm3 and the weight is only about 270 ng which possesses a Miura-ori patterns joined together (one with higher crease
volume filling fraction of 1.5%. The numerical calculation which stiffness than the other) in 3D by geometric transformation (180
was calibrated based on the fabricated sample shows a rotation). The 3D zig-zag shaped assembly requires equal spine
remarkable figure of merit. The ratio of bulk modulus to shear angles between the 2 unit cells, imparting a distinct kinematic
modulus is made realistically as large as 1000. Further study constraint on the deformation of the metamaterial that has not
pointed that if the critical dimensions could be reduced to 0.1 μm existed in planar tessellations of origami metamaterials.
while maintaining other parameters, the pentamode figures of Experimental observations demonstrate that the 3D stacked
merit would exceed 10 000. After that Kadic also theoretically and origami that the energy barrier of the extension switch could be
experimentally proposed a class of modified pentamode increased without significant change in the barrier of the
metamaterials and laminate heterostructures for which the opposite compression switch. This results in an asymmetric
effective parameters bulk modulus and mass density can be energy barrier, and via strengthening the kinematic constraint, it
independently adjusted over a large range.[349] By using three- is possible to achieve a mechanical diode effect. This implies that
dimensional printing technique, macroscopic polymer-based this static non-reciprocity in origami could be implemented in
Figure 16. Examples of fabrication processes to produce core-shell, hollow, and glassy carbon nanolattices. a) A negative polymer template is initially
fabricated to be used a mold using a fabrication method (e.g., two-photon lithography). Electroplating is then employed to fill in the mold with a metal
such as Cu. The polymer is subsequently etched away and the resulting metal structure is coated with a thin layer of another material to form the
composite structure (e.g., by Plasma-Enhanced Chemical Vapor Deposition (PECVD)).[230] b) The polymer scaffold is synthesized. A thin coating layer is
then conformally coated onto the polymeric structure. The edges of the composite structure is removed by Focused Ion Beam (FIB) to expose the
polymer within each strut. An etching technique is used to etch the exposed polymer scaffold to finally produce the hollow nanolattice.[229] c) Pyrolysis of
a polymer nanolattice to produce glassy carbon nanolattice with significant volumetric reduction.[14]
several novel applications such as motion rectification and wave via increasing the number of triangular patterns (Figure 17c, d).
propagation control.[65] Similarly, Fang et al. have recently made By adopting joints that allow combined deformation, such as
use of 3D tessellation to propose the single-collinear (SC) pattern twisting and compression, the properties of the metamaterial
(Figure 17a), which can be derived from the Miura-ori pattern, to could be adjusted depending on the directions of external load
achieve self-locking in cellular origami metamaterials. This applied. For instance, upon uniaxial compression of the
provides a pathway to attain large deformation via folding of non- metamaterial with angles greater than a critical value, it will
rigid creases while allowing for programmable stiffness at exhibit high stiffness. However, by subjecting the metamaterial
different stages of deformation in 3D origami (Figure 17b).[41] surface to shear stress and axial stress through the inclusion of
Zhai et al. studied the triangulated cylinder pattern and altered rotational forces, the joints deform and changes the crease angle.
its crease angles to achieve an origami metamaterial with on- As the angle decreases beyond the critical value, the meta-
demand deployment and collapse in addition to tunable stiffness material will exhibit low stiffness under uniaxial compression.
Figure 17. Examples of 3D cellular origami-inspired metamaterials. a) Schematic illustration of a single-collinear (SC) unit cell based on an asymmetric
Miura-ori pattern showing its self-locking behavior upon compression.[41] b) Finite Element Analysis of a prototype 3D SC unit cell throughout the
various stages of deformation, namely, pre-locking, locking, and post-locking.[41] c), d) Origami-inspired metamaterials based on the triangulated
cylinder pattern. It demonstrates that by adjusting the crease angle of the unit cells, different deployability and collapsibility could be achieved.[69] e)
Deployment and retraction of a zipper-coupled tube origami-inspired metamaterial based on the Miura-ori pattern.[70]
They have demonstrated that its design principles could be electrodes 10–100 times thinner.[228] Similar approaches that
applied to obtain nonmonotonic strain paths attributed to the utilize DIW and supercritical or freeze-drying process to
triangular patterns and unique kinematic constraints as well.[67] fabricate highly porous architectures, such as the GO/carbon
Filipov et al. have developed a zipper-coupled tube origami- nanotube composite aerogels,[353] GO/geopolymer aerogels,[354]
inspired metamaterial based on the Miura-ori pattern, which etc. have been known to exhibit desirable functional character-
allows for reversible deployment while simultaneously retaining istics while retaining excellent mechanical properties.[355]
high global stiffness (Figure 17e).[68] This was achieved by using Besides mechanical metamaterials fabricated by DIW, other
2 stacked Miura-ori tubes, where 1 of the tube is rotated and 3D printing methods such as SPPW and TPL have also been
connected with the other one in a zig-zag (zipper) manner. The used to develop micro/nanolattices for energy storage applica-
zipper geometry results in an anisotropic stiffness and tions, for example, supercapacitors and batteries. For example,
deformation behavior, where it could be exhibit high stiffness Xu et al. developed a hollow Au microlattice as positive electrodes
in a certain direction, while possessing relatively low stiffness in for Li–O2 batteries by initially fabricating an architected
the other to allow for deployment of its bistable unit cells. polymeric scaffold by SPPW, followed by depositing a thin layer
of Au through sputtering and electrodeposition prior to chemical
etching to remove the polymer (Figure 18d–f).[229] Xia et al.
4.2. Mechanical Metamaterials for Functional Applications performed in-situ lithiation and delithiation of a high strength
Cu-Si core-shell nanolattice which could accommodate approxi-
Mechanical metamaterials have the potential to not only produce mately 250% expansion of Si upon lithiation. This was done by
engineering materials with desirable and tunable mechanical developing a negative polymer template or mold of a stretching-
properties, but also exhibit other unique properties for dominated architecture and electroplating Cu into the mold.
functional applications. For instance, they have immense Subsequently, the polymer was removed by chemical etching
potential to be applied in the energy storage and biomedical and the Si outer shell was deposited via plasma-enhanced CVD
industries. In electronics, employing optimally structured (PECVD) (Figure 18g, h).[230] A hybrid solid electrolyte consisting
metamaterials in electronics as supercapacitors, battery electro- of an ordered bicontinuous 3D microarchitecture of ceramic and
des or solid electrolytes provides a solution to conventional polymer have also been developed by Zekoll et al. that could
design constraints. Large pore volumes for mass transport and potentially address one of the crucial challenges faced for
surface areas to maintain high charge-discharge rates are producing all solid-state batteries, which is developing an all-
typically desirable. However, stochastic cellular materials solid-state electrolyte with adequate ionic conductivity while
typically exhibit poor mechanical performance. Mechanical maintaining mechanical robustness.[237] This was achieved by
metamaterial has the potential to decouple this trade-off between the initial synthesis of a 3D architected polymer scaffold by TPL.
pore volumes and mechanical robustness by maximizing the A structured ceramic lithium ion conductor Li1.4Al0.4Ge1.6
usable pore volume through an engineered structure design, (PO4)3 (LAGP) microchannel was then produced by negative
making it possible to explore other kinds of material that templating of the polymer scaffold. The thermal heating to sinter
traditionally suffers from undesirable mechanical properties. the LAGP powder removes the polymer scaffold and the empty
Zhu et al. used DIW-based 3D printing to fabricate micro-channels within the ceramic template was filled with
hierarchical graphene-based aerogels which possess relatively polymer (polypropylene melt or liquid epoxy) through resin
high stiffness while being extremely lightweight due to its highly impregnation to finally form the solid-state electrolyte. Other
porous nature (Figure 18a–c).[352] Its architecture enables it to applications of mechanical metamaterials in electronics also
exhibit superior mechanical properties, with large surface areas include the manufacture of sensors,[356] actuators,[357] and
and a Young’s modulus of an order of magnitude higher than filters,[358] which typically involve the use of highly compliant
bulk graphene materials with similar geometric densities. topologies such as origami, kirigami-inspired structures and
Initially, a tailored graphene oxide (GO)-based ink which consist other auxetics. For instance, Ning et al. synthesized 3D
of GO filled with silica nanoparticles was extruded through a mesostructures by compressive buckling of 2D kirigami patterns
micro-nozzle by DIW to form the 3D structure in isooctane, piezoelectric thin-film micro-actuators for vibratory excitation
which prevents drying while printing. Subsequently, the and precise control in various electronic and biomedical
microlattice structure was supercritically dried to remove the devices.[359]
liquid inside, followed by carbonization under an inert In the biomedical field, micro/nano-architected and origami
atmosphere and chemical etching to remove the silica fillers. cellular structures could serve as bio scaffolds to promote the
The resulting hierarchical structure shows excellent mechanical organized growth of cells, tissue constructs, deployable
recoverability, with less than 5% plastic deformation after angioplasty and esophageal stents, or artificial implants with
uniaxial compression at 90% strain. Similarly, Zhu et al. have tunable mechanical properties. Cell culturing in a 3D environ-
employed a similar approach to fabricate an architected ment has dated back in the early 20th century by Ross Harrison,
graphene composite aerogel supercapacitor, consisting of and extensive studies on understanding the behavior of cells and
reduced GO and graphene nanoplatelets (GNPs), which have benefits of a 3D environment have been conducted since then.
been demonstrated to exhibit superior electrochemical perfor- Bio-scaffolds generally need an interconnected pore network for
mance owing to its high porosity. The synthesized macro-scale the growth of cells and flow transport of nutrients or metabolic
electrodes displayed remarkable capacitive retention (ca. 90% waste. However, it has been difficult to systematically and
from 0.5 to 10 A g1) and power densities (>4 kW kg1) that quantitatively control the topology of these 3D scaffolds until
equal or exceed those of previously reported devices made with recently. One of the most versatile techniques to synthesize 3D
Figure 18. Examples of architected cellular materials for energy storage applications. a) Optical image of a graphene-based aerogel microlattice
fabricated by Direct Ink Writing (DIW).[352] b), c) Scanning Electron Microscope (SEM) images of the hierarchically porous internal structure of the
graphene aerogel microlattice.[352] d) Optical image of a 3D hollow Au microlattice battery electrode.[229] e), f) SEM images of the internal structure of the
hollow microlattice.[229] g) Illustration of a core-shell nanolattice Li-ion battery electrode consisting of a SI core and Cu shell.[230] h) In-situ lithiation of the
Cu-Si core-shell nanolattice exhibiting 250% volumetric expansion of Si.[230]
bio-scaffolds with well-defined topologies that mimic the have also fabricated 3D micro-cages using TPL to disseminate
structure and length scale of natural 3D environments have between non-tumorigenic and tumorigenic human breast cells
been to use additive manufacturing techniques. These techni- based on their metastatic potential and the invasiveness of the
ques also offer the unique advantage of being able to cater to a cell lines at various pore sizes.[236] Accardo et al. utilized TPL
patient’s specific requirements, allowing the optimization of to synthesize woodpile-like poly (ethylene glycol) diacrylate
mechanical and biological properties. Materials used to fabricate (PEGDA) architectures and colonize it with neuro2A cells to
these scaffolds typically needs to be non-toxic, biocompatible, form neuritic extensions or interconnections.[360] Highly
and ideally meets the requirements provided by the food compliant tetrakaidekahedral nanolattices with tunable stiffness
and drug administration (FDA). Polymers, either natural or made of a UV curable polymer (IP-Dip) coated with Ti, W, and
synthetic, are commonly used, although glass, ceramics, and TiO2 were fabricated by Maggi et al.[235] These nanolattices were
metals are sometimes used as well, especially when the seeded with osteoblast-like cells (SAOS-2) and their mechano-
mechanical integrity is of a crucial concern (e.g., implants). sensitive responses were investigated based on its mineral
Figure 19a–c exhibit cardiomyocytes cultured in a fibronectin- secretions, intracellular f-actin and vinculin concentrations after
functionalized 3D architected scaffold made of OrmoCorp, a UV cell culturing. Engineered tissue constructs made of vasculature,
curable and biocompatible hybrid polymer.[234] Spagnolo et al. multiple types of cells, and extracellular matrix (ECM) have also
Figure 19. Architected cellular structures for biomedical applications. a), b) Scanning Electron Microscope (SEM) images of 3D printed cell scaffolds
made of photopolymer using Two Photon Lithography (TPL).[235] c) 3D reconstruction of a laser scanning microscope (LSM) confocal image stack
showing the culturing of Cardiomyocytes cultured in a fibronectin-functionalized 3D scaffold.[234] d), e) Hybrid metallic meta-implants consisting of both
auxetic (negative Poisson’s ratio) and conventional (positive Poisson’s ratio) 3D architectures manufactured using Selective Laser Melting (SLM).[233]
been realized through multi-material DIW by Kolesky et al.[361] region with positive Poisson’s ratio will experience compression
Mechanical metamaterials can also be used to create arterial or and cause the region with the auxetic structures to undergo
esophageal stents owing to its unique deformations.[46,362,363] expansion. This will result in the compression of the
For instance, Ali et al. designed and manufactured an auxetic surrounding bone along both implant contact lines, preventing
and biocompatible polypropylene film based on the rotating- wear particles to enter the interface while promoting bone
squares geometry which could be wrapped around a cylindrical growth. These works demonstrate the potential of architected
rod to form a tubular stent. This could be used for the palliative cellular materials in synthesizing structured biomaterials with
treatment of esophageal cancer and prevention of dysphagia desirable mechanical properties and topology to provide a
via expansion of the tubular stent arising from it auxetic favorable environment for cell growth, allowing for more
properties.[362] Similarly, Gatt et al. proposed a second-order effective and safer prostheses to be made.
hierarchical stent derived from the rotating-squares geometry, In addition to functional applications in the energy storage
which could enhance the magnitude of Poisson’s ratio, and biomedical industries, these metamaterials have also been
consequently reducing inflammation due to reduced contact demonstrated to have potential applications in the field of
area. Owing to the relieved pressure on the swelling area, the acoustics, photonics, and thermal management. For instance,
hierarchical design could potentially be used in skin grafts as the effective bulk modulus of pentamode metamaterials, which
well.[75] Other recent progresses include a rationally-designed was introduced in the previous section, can be tuned which
hip implant (Figure 19d, e) which combines both auxetic means the speed of wave in material is possible to be
(negative Poisson’s ratio) and conventional honeycomb (positive manipulated. Chen et al.[224] proposed a practical latticed
Poisson’s ratio) structures to decrease the probability of a bone pentamode acoustic cloak. The acoustic cloak was assembled
implant interface failure by minimizing the chance of wear by pentamode lattice made of single-phase solid material which
particles entering the enclosed space (Hoffman’s criterion) and could reroute acoustic wave round an obstacle. Layman et al.[225]
mechanically stimulating bone growth to enhance fixation.[233] presented an anisotropic pentamode design formed by honey-
They made use of SLM to 3D print these hybrid meta-implants comb microlattice. The pentamode structure design could be
with biomedical-grade titanium alloy Ti6Al4V-ELI. The implant customized by altering the honeycomb lattice geometry which
is designed in such a way that during mechanical loading, the results in the realization of material properties in the physical
space as required by coordinate transformations. It was absorption capabilities.[217] Similarly, Roper et al. developed
demonstrated anisotropy in stiffness could be achieved and polymeric heat exchangers with optimized architectures via SLA
exceed 3 orders of magnitude, which could be rationally tuned and SPPW to initially create the sacrificial scaffolds, followed
for transformation acoustic applications. A cellular metamaterial by coating with parylene and chemical etching of the scaffold
with both negative Poisson’s ratio and tunable acoustic band gap to form enclosed micro-channels.[216] This allows for heat
has been developed recently by Chen et al. via tailoring its exchanger design which decouples the traditional coupling
geometric parameters such as length of unit cell, porosity and between thermal performance and the thermal conductivity of
aspect ratio of the individual pores.[364] Yu et al. have also the solid material. Dou et al. have also investigated the potential
developed a stimuli-responsive acoustic metamaterial based on of hollow alumina nanolattices as mechanically robust insulators
an octet-truss topology made of ferromagnetic nanoparticle- with ultralow thermal conductivity, high stiffness and damage
filled elastomer.[226] The effective modulus of the synthesized tolerance. Its insulative properties have been demonstrated to be
magnetoactive acoustic lattice could be reversibly switched comparable to that of aerogels, which are typically the primary
between positive and negative through elastic buckling which choice of material with ultralow thermal conductivity, but
occurs as the applied magnetic field is varied. This strategy exhibits a specific elastic moduli of nearly 2 orders of magnitude
which could extend the 2D phase space to 3D has the potential to higher.[218]
be used for a wide variety of novel acoustic devices with rapid, These strategies demonstrate the versatility of mechanical
remote, and switchable acoustic transportation, refraction, metamaterials which combines the benefits of architecture and/
imaging, and focusing. or size effect with a wide variety of material constituents at
Architected 3D photonic crystals have also been made in the different length scales in providing a novel route to synthesize
recent years. For example, Ergin et al. have created a 3D optical functional materials with unprecedented and superior proper-
invisibility cloaking structures using a modified dielectric ties. This also allows us to alter the properties of materials
photonic crystal via TPL.[219] Edagawa et al. have proposed the conventionally known to exhibit unexpected mechanical proper-
photonic amorphous diamond” (PAD), which consisted of a ties despite possessing huge potential for a specific application,
cellular network of dielectric rods with a diamond-like local enhancing its potential for multifunctional applications.
tetrahedral configuration, for terahertz applications.[221,365]
Through terahertz time-domain spectroscopy, they have discov-
ered that the photonic crystal formed a photonic bandgap at
5. Conclusions and Perspectives
around 0.45THz. Chernow et al. have also fabricated polymeric
photonic crystal nanolattice using octahedron unit cells, which The extensive studies conducted due to the emergence of
were able to cause a 2.2 μm wavelength shift when compressed mechanical metamaterials has allowed us to infiltrate into
to 40% strain, from 7.3 to 5.1 μm.[220] Liu et al. utilized previously inaccessible regions in the conventional material
irradiation-induced buckling in kirigami patterns to develop 3D property space and breach the intimate coupling between
nano-structures from 2D precursors via FIB and subsequent materials’ properties. Despite the limited data available which
global ion beam irradiation, resulting in giant intrinsic optical subjects the principles discussed here to some uncertainty owing
chirality as opposed to its 2D counterparts. This method provides to certain experimental constraints, the foundation that has been
a one-step quick process to manufacture versatile 3D structures laid thus far would undoubtedly contribute to the discoveries of
with nano-scale features for plasmonics, nanophotonics, more novel metamaterials with intriguing properties. The rapid
MEMS/NEMS, etc.[80] growth in advanced manufacturing techniques, especially 3D
Architected cellular cores have been used for thermal printing, has enabled the fabrication of intricate features
management as well. Cold plates, heat pipes and exchangers at various length scales that have not been possible using
are some of the most crucial components in thermal manage- conventional casting or molding methods. Among the various
ment, particularly in high-performance cooling systems. The techniques made available in the recent years, TPL has been
incorporation of micro-scale architectures has enabled the mostly responsible for the success of mechanical metamaterials
enhancement in its performance, such as increased heat transfer at the nano-scale, particularly nanolattices, while SPPW and
rate, reduced mass, energy input requirements, and temperature PμSL have been mainly used for micro-scale architectures.
drop. Improvement in efficiency is also expected due to the Although these techniques primarily involve the fabrication of
enhanced heat transfer per unit area and inverse scaling between polymeric scaffolds, recent advances have made it possible to
surface area-to-volume ratio with the overall dimensions of the synthesize metallic or ceramic metamaterials as well. Combined
device.[32,212] Valdevit et al. has investigated and compared the with different post-processing methods, these micro/nano-
topological configurations of various heat sinks and showed that lattices have been known to exhibit remarkable and unique
periodic architectures such as truss cores exhibit superior mechanical properties such as ultrahigh specific strength,
cooling performance in comparison to that of textiles and resilience, negative Poisson’s ratio, high bulk modulus-to-shear
randomly porous foams.[213] Heat exchangers with enhanced modulus ratio, chirality, and static non-reciprocity. Furthermore,
heat transfer properties have also been previously reported.[214– it is also possible to tailor the deformation modes of mechanical
217]
For instance, Maloney et al. have fabricated cross-flow heat metamaterials to cater specialized applications. These distinctive
exchangers made of Ni hollow microlattices, by sacrificial features found in multi-scale mechanical metamaterials could be
templating of a polymer core, to demonstrate the multi- coupled with the intrinsic properties of its constituents to further
functionality of architected cores in not only increasing the enhance its multifunctionality across a wide range of applica-
heat transfer performance, but also its load-bearing and energy tions, including but not limited to energy storage, biomedical,
acoustics, photonics, and thermal management. The increasing applications in the future. Pertaining to the testing and
exposure and apparent growth of this field would surely result in characterization of metamaterials, increasing the speed of 3D
other novel applications to be explored. tomography at various length scales to the point where it could
While fabrication techniques that could exploit both the benefits be coupled with in-situ mechanical testing platforms will be
of architecture and size effect have mainly been applied to crucial to fully understand the deformation mechanisms of
mechanical metamaterials at the micro- or nano-scale, tremen- metamaterials. This would not only be useful for the investiga-
dous effort have been put to address the scalability of these tion of mechanical properties but could also be used for
processes, especially since the past decade. As of now, powder- functional property change as the metamaterial is subjected to
based 3D printing techniques such as SLS and SLM have perhaps various external conditions. Mechanical metamaterials have
been the most successful in terms of its use for industrial certainly attracted increasing interest over the past few years and
applications. However, we have yet to achieve the surface finishing based on the foundation that been laid out thus far, it is expected
quality provided by traditional casting or molding nor the that this field will yield more breakthroughs in the near future.
dimensional accuracy provided by high-end light-based 3D
printing such as TPL with these methods. Therefore, the
paramount challenge in this field has been to develop a scalable
solution to proliferate nano-scale features into macro-scale
Acknowledgements
materials. Some of the potential routes to achieve increased JUS, LG, XL, and YL gratefully thanked the funding supports from
scalability include a step-wise fabrication using optical techniques Shenzhen Science and Technology Innovation Committee under the grant
such as TPL, where structures are printed through a combination JCYJ20170413141157573. Part of this project was supported by the
Research Grants Council of the Hong Kong Special Administrative Region
of multiple intersecting build areas. Due to the repeating nature of of China (GRF No. CityU11216515) and City University of Hong Kong
most micro/nanolattice structures, parallelization techniques for (Project Nos. 9667164 and 9667153). NXF and HD acknowledged support
high throughput fabrication could also be implemented. This by the U. S. Army Research Office through the Institute for Soldier
could be done via beam splitting and/or concurrent synthesis with Nanotechnologies at MIT, under Contract Number W911NF-13-D-0001,
multiple beams in different areas that eventually intersect with and the support from Grant No. 2016284 from the United States-Israel
each other to form a single part. Hybrid techniques which combine Binational Science Foundation (BSF).
The manuscript has been modified after online publication.
two or more different AM techniques, such as extrusion-based
with light-based AM, might also help to achieve improved
scalability while preserving nano-scale features. Self-assembly of
these metamaterials through the input of an external energy might Conflict of Interest
also be feasible. On the other hand, the integration of AM with
The authors declare no conflict of interest.
subtractive techniques (e.g., laser cutting) might allow current AM
methods with the capability to produce macro-scale structures to
achieve unprecedented resolution. However, the implementation
of these techniques is plagued with several technological Keywords
challenges, such as the possibility of introducing macroscopic
mechanical metamaterial, microlattice, nanomanufacturing,
flaws into the overall part which could nullify the benefits of size- nanomechanics, origami, structural materials, 3D printing
effects. The incorporation of imaging and auto-correction
techniques into micro-/nano-scale fabrication methods could
Received: August 11, 2018
potentially prove to be a pivotal point in the field. Furthermore, the
Revised: November 16, 2018
limited selection of materials remains to be a challenge. The
Published online: January 4, 2019
development of new engineering materials, especially those that
enhance the sustainability of AM processes is expected to be of vital
importance in the scalability of production from the laboratory to
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