Complex Selective Manipulations of Thermomagnetic Programmable Matter

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OPEN Complex selective manipulations


of thermomagnetic programmable
matter
Josu Irisarri 1, Iñigo Ezcurdia 1, Xabier Sandua 2, Itziar Galarreta‑Rodriguez 3,
Jose Ignacio Pérez‑Landazabal 3 & Asier Marzo 1*

Programmable matter can change its shape, stiffness or other physical properties upon command.
Previous work has shown contactless optically controlled matter or magnetic actuation, but the
former is limited in strength and the latter in spatial resolution. Here, we show an unprecedented level
of control combining light patterns and magnetic fields. A mixture of thermoplastic and ferromagnetic
powder is heated up at specific locations that become malleable and are attracted by magnetic fields.
These heated areas solidify on cool down, and the process can be repeated. We show complex control
of 3D slabs, 2D sheets, and 1D filaments with applications in tactile displays and object manipulation.
Due to the low transition temperature and the possibility of using microwave heating, the compound
can be manipulated in air, water, or inside biological tissue having the potential to revolutionize
biomedical devices, robotics or display technologies.

Programmable matter can change shape, density, moduli or other physical properties in a programmatic w ­ ay1.
2
These changes are controlled externally or triggered by embedded sensing and processing in the m ­ aterial . The
main two approaches towards implementing programmable matter are: modular r­ obots3, which provide more
intelligence; and external a­ ctuation4, which yields a higher spatial resolution and scalability. Programmable
matter holds ground-breaking applications in engineering and medical fields, but the granularity that can be
achieved in its manipulations is still significantly limited.
Light has been used as an external actuation method. Materials combined with a­ zobencenes5 are actu-
ated when illuminated. For example, triggering movement when a reflective or opaque object approaches the
­material6, or enabling locomotion on filaments and cylinders when illuminated with dynamic light p ­ atterns7.
On the other hand, the heat generated by light can move small objects on the water surface due to temperature
­gradients8 or change phase in shape-memory a­ lloys9. Actuation with light or its thermal effect has high spatial
resolution given the existing technology to project images, yet the actuation strength is relatively weak and after
actuation, the whole material returns to its initial state or retains a non-reversible state. Moreover, light cannot
pass through opaque materials.
Magnetic fields are another way of controlling matter from a distance. A flexible thread of polymer contain-
ing magnetic powder can be steered remotely to navigate contorted e­ nvironments10, sheets of flexible materi-
als embedded with ferromagnetic or magnetic particles can be translated and flexed in a controlled way for
­locomotion11,12, a carpet made of magnetic cilia can be actuated to control the objects that are on top of i­ t13, and
magnetic slime can be moved magnetically to trap and transport other o ­ bjects14. Magnetic actuation is strong
and can pass through non-metallic materials yet it is not possible to have high-spatial resolution since magnetic
fields do not remain focused at a distance. For better control, the magnetic attraction or repulsion on the mate-
rial can be modulated by heating it up towards its Curie temperature, either using ­light15 or electromagnetic
­induction16, yet these methods are applied on the whole surface not allowing fine manipulation. Liquid metal
­ roplets17 by external magnetic fields, and when they are combined in a magnetorheological
can be translated in d
slurry it can also change ­stiffness18, serving as dynamic electrical connection in reconfigurable circuits.
Here, we show unprecedented levels of control manipulating matter using a combination of thermal spatial
patterns and magnetic actuation on a composite material made of a matrix of low-temperature reversible thermo-
plastic (Polycaprolactone, PCL) mixed with ferromagnetic powder (iron particles), see “Methods” “Compound
mixing”.
Thermoplastics have been mixed before with iron powder for tuning its thermal ­conductivity19, electrical
­resistance20 or oxygen a­ bsorption21. In the context of programmable matter, the combination of magnetic and

1
UPNA ISC, UpnaLab, 31006  Pamplona, Spain. 2Physics Department, UPNA, 31006  Pamplona, Spain. 3Science
Department, UPNA INAMAT2, 31006 Pamplona, Spain. *email: [email protected]

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Figure 1.  Manipulations on a ferromagnetic thermoplastic using thermal patterns and magnetic fields. (a) Hot
air makes the centre of a filament malleable, a magnetic field pulls one side of the filament that bends along the
heated area, on cool down the filament is solidified. (b) A laser heats up specific points on a sheet, a magnetic
field attracts those points upwards, on cool down the raised points are fixed and can be pressed without
deformation. (c) A 2D pattern is illuminated into a sheet of material, when a magnetic field is applied, the
heated areas rise and on solidification they become embossed. (d) A blob of material rises into a column, a point
on the column is heated and a secondary branch is pulled from it. (e) Microwaves can heat the material when it
is inside an optically opaque material for example to expand its container or actuate it.

thermal actuation has been shown for this kind of ­compound22,23, yet the manipulations were only applied to
2D sheets and the heat was applied to the whole material, limiting significantly the types and complexity of the
manipulations.
In our presented manipulations, the material is solid at room temperature (25 ◦ C) but becomes malleable
beyond 50 ◦ C by the application of heat on specific locations. The heat can be applied globally, with an IR lamp;
at a localized area, utilizing hot air guns; with spatial patterns, using a mask on collimated light; at a focal spot,
using focused halogen lamps or lasers; and inside opaque materials, with microwave radiation (see “Methods”:
“Thermal sources”). Then, a magnetic field attracts the Fe particles that are embedded within the matrix, drag-
ging the malleable parts of the PCL with them. The material solidifies when it cools down at room temperature,
being this process repeatable. Different applications ranging from the formation of Braille code to sculpting
figures are enabled using spatially complex thermal patterns applied on 1D filaments, 2D sheets or 3D blocks
(see Supplementary Movie 1). The basic principle is shown in Fig. 1.
A qualitative model of the working principle is shown in Supplementary Movie 2. The following equations
were combined in a connected particle time-domain simulation to inform the experiments  presented
 in the
paper.The H-Field generated by the magnet is approximated as a d ­ ipole24: H(r) = 4π
1 3r̂(m·r̂)−m
r3
where r is the
vector from the dipole to the point in the field, and m is the magnetic moment of the dipole. This magnetic force
that the H-field exerts on an iron particle is calculated ­as25: Fm = µ0 Vp Mp ∇ Hp where µ0 is the Vacuum

magnetic permeability,Vp is the particle volume and Mp is the magnetization of the particle calculated ­as25. The
distribution of the heat inside the material is modelled using the common heat equation ∂u ∂t = α�u where α is
the thermal conductivity. The viscosity of the material determines its shear displacement for a given force
F = µA uy where µ is the viscosity, A is the area, and uy is the rate of shear deformation; for a thermoplastic, its
viscosity ( µ ) decreases logarithmically with t­ emperature26.

Results
Characterization of the material.  Multiple samples with different proportions of iron particles were
created and moulded into cylinders (see “Methods”: “Compound mixing”), mechanical and magnetic charac-
teristics were measured. The samples were labelled from S10 (10% of iron in volume) to S50 (50% iron volume),
adding iron powder beyond 50% volume made the sample brittle and not able to maintain its structure.

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Figure 2.  (a) Temperature on the top of the samples over time when placed on a heated bed at 50 ◦ C, the heat
is removed after 60 min; with color (b,c) thermal images. (d) Temperature over time at the side of the samples
when a focal spot is applied at the center, the heat is removed after 20 min; with color (e,f) thermal images. (g)
Magnetic pulling force on the samples.

Thermal conductivity was monitored through the cylinders of 5 cm diameter and 3 cm thickness (Fig. 2a)
when they were placed on a closed-loop heated bed at 50 ◦ C (Fig. 2b,c). The larger the iron content, the greater
the thermal conductivity through the material, temperature was measured on the top surface of the cylinders.
Surface conductivity was also monitored (Fig. 2d–f), the lower the content of iron, the higher the temperature
reached and the longer it took to cool down; this may happen because the heat cannot be distributed through
the material. More details are in “Methods”: “Thermal measurements”. The light intensity can be regulated to
raise the temperature of the material at different rates (see Supplementary Image 7).
Magnetic pulling forces were measured on the different samples and are shown in Fig. 2g. The larger the
iron content, the stronger the magnetic force. The maximum magnetic attraction distance was similar for all the
samples ( ≈ 6 cm) since samples with more iron volume were more strongly attracted but also weighted more.
More details are in “Methods”: “Magnetic measurements”. Additional characterization (Hardness Shore and
Tensile Tests as well as Microscopic, confocal and SEM images) are available in Supplementary Figs. 8, 9, 10, 11,
12 and 13 respectively.
The material was homogeneous in colour after preparation and actuation. Furthermore, the density of differ-
ent parts showed a very small deviation (SD = 0.006 g/ml) as is shown in Supplementary Image 6. This indicates
that the powder had a homogenous distribution even after actuation and that no agglomeration of powder
occurred after the magnetic field actuation.

Basic manipulations.  Basic operations on the material are performed by heating up a specific area, attract-
ing that area with a magnetic field and then cooling it down by passive dissipation or actively with a cold air jet.
The material can be employed in different dimensionalities: 1D filament, 2D sheets and 3D slabs.
When the material is at solid state, a magnetic field can translate it along surfaces using regular magnetic
attractive manipulation. Since we used ferromagnetic Fe particles, the compound is always attracted by the

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Figure 3.  Basic manipulations. (a) Bending and unbending. b) Stretching and contracting. (c) Splitting. (d)
Merging. (e) Rising. Scale bars are 3 cm.

magnet. Precise and selective control is possible. Using two magnets, rotation of elongated pieces of material was
achieved. Applying heat can melt and flatten specific parts of the material or the whole piece if applied globally
either with magnetic forces pulling from below or by the action of gravity. These basic manipulations are shown
in Supplementary Fig. 5.
Bending of elongated pieces can be achieved at a targeted location by applying focused heat on the desired
pivot point, then applying a magnetic field above the pivot; the other part can be held in placed: by its own
weight if it is large enough, by another magnet or by sticking it with heat; unbending operations are performed
with the reverse process (Fig. 3a). Stretching and contraction is accomplished when both parts (above and
below the heated area) are moved by separating or approximating them respectively (Fig. 3b). If the solid parts
are separated further, the heated malleable part breaks and the material splits into two parts (Fig. 3c). Joining
separated pieces can be performed by heating them on the target joining areas, and then pushing these areas
together (Fig. 3d). Rising of a part can be achieved by heating up the whole sample and then applying a magnetic
field from above (Fig. 3e).
Heating the surface of the material can be achieved in 1 min with light, heating the whole piece can be done
in 10 min. Bending was performed at 5 ◦/s, the stretching and contracting manipulation took 10 s, the duration
was similar for splitting. To achieve full separation into two parts, a minimum distance of 5 cm. was required.
The rising speed was 5 mm/s, it is possible to go faster but precise control is needed to avoid that the material
gets into the magnet. The maximum height was 10 cm, longer branches can be obtained but they needed to be
cooled down externally to avoid collapse.

Complex manipulations.  Different letters can be created starting from a single strand of filament by com-
bining basic operations. The filament is split into the different segments that will make each letter. The separated
parts were bent at targeted positions at specific angles. Then, some segments were joined together. Each letter can
be moved as a whole solid afterwards. The letters, S,M,A,R,T were created using this process (Fig. 4a).
Arbitrary patterns can be raised in a sheet by applying light patterns to make it malleable at specific posi-
tions. Then, a magnetic field from above, rises the malleable areas. Braille patterns (Fig. 4b) and the contour of
the letter M (Fig. 4c) were embossed on sheets. This process is reversible by applying heat on the whole surface
for flattening it out.
An organic tree shape was created by rising a blob of material into a main trunk, then sub-branches were
extruded (Fig. 4d). A sculpture of a sea creature was created from a lump of material. Firstly, it was flattened by
melting. Then the general shape of the tail, neck and fins was stretched. Secondly, spikes were risen along the
tail. Thirdly, the low-neck was heated and then raised by pulling from the top. Finally, the end part of the neck

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Figure 4.  Complex manipulation. (a) Forming letters with 1D filament. (b) Reversible Braille patterns on a
sheet. (c) Embossed letter M on a sheet. (d) Branching. (e) Sculpting in 3D. Scale bars are 3 cm.

Figure 5.  Use cases. (a) A hook to grab a small object. (b) A larger hook to drag a heavier object, can pull
up to 20 kg. (c) Operation under water. (d) Lifted column as a support structure. (e) Filament sticking to
separated places to connect them. (f) Filaments stacked at different distances for selective filtering. (g) Heating
of the material inside a container using microwaves for being able to expand and contract it dynamically, after
solidification it maintains the container expanded. Scale bars are 3 cm.

was moulded into a head by bending it down and raising two small antennas (Fig. 4e), we note that all these
steps were done from a distance.

Use cases.  Flexible filaments doped with magnetic powder can be used to navigate through contorted
­environments10, here we can also control which parts of the filament become flexible or rigid by heating them
up, this enables to use the filament as a hook to grab objects in air (Fig. 5a,b) or water (Fig. 5c).
The mechanical properties of the thermoplastic enables the material to work as a support for structures
(Fig. 5d). When the material is heated up beyond 80 ◦ C and then cooled down it sticks to different surfaces, this
can be used to connect separated areas (Fig. 5e) and filter passing objects (Fig. 5f).
The material can be heated up also when it is inside optically-opaque media using microwaves. A 2.45 Ghz
magnetron heated up the material making it malleable while it was inside a lung simulator balloon. Then, with

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Samples S10 S20 S30 S40 S50


Fe volume (%) 10 20 30 40 50
PCL volume (%) 90 80 70 60 50
Fe (g) 16.81 33.61 50.42 67.21 84.03
PCL (g) 22 19.5 17.11 14.66 12.22

Table 1.  Iron and PCL proportions in volume and weight for each sample.

a magnetic field it could be expanded and shrunk in a controlled way, when the material solidified, it kept the
balloon expanded (Fig. 5g).

Discussion
The magnetic fields have a limitation on their reach of ≈ 6 cm, yet the employed magnets were regular neodymium
cylinders. Stronger magnetic fields from specialised equipment would provide a larger reach.
Heat diffusion is necessary for making the material malleable beyond the surface where the light illuminates
the material. However, diffusion makes the thermal patterns less sharp and limits the achievable steepness on
surface deformations. Materials with less concentration of iron have less conductivity through the material and
get hotter on the surface, thus are better suited for surface manipulations like Braille codes. Compounds with
more iron are more adequate for manipulations on the bulk (e.g., bending, splitting, rising or melting). Microwave
heating can be used for bulk heating even if thermal conductivity is low because it penetrates on the material,
whereas light-based methods or air are more suited for surface heating.
Homogeneous compounds were obtained by mixing the thermoplastic polymer with iron particles. Given the
size of the particles and viscosity of the material, the compound retained its uniformity after multiple manipu-
lations (i.e, the particles dragged the plastic with them) on the same piece. Oxidation of the iron particles or
change of colour was not observed in the materials throughout the experiments, even on the samples that were
immersed in water.
The magnetic fields where controlled in a close-loop manner by moving and rotating the magnets according
to the visual observation of the material reactions. However, heating was applied in open-loop, more control
could be obtained in the thermal patterns if they were applied in close-loop with a thermal camera.
The employed thermoplastic (PCL) is biocompatible, iron particles (or their oxide) are of common use in
medical applications. Additionally, microwave radiation can heat up iron particles without heating up signifi-
cantly the surrounding biological t­ issue27. This makes the compound viable for operations inside the human body
manipulating it from the outside, for example along the digestive tube or upper respiratory tract.
In this paper, we focused on the mechanical manipulations that are only possible due to the thermomagnetic
actuation, different functionalizations can be added to the material. For example, adding silver compounds to
make it conductive and functional in reconfigurable circuits, or antibiotic microcapsules at the centre that get
released when the material is split.
Remote manipulations of unprecedented complexity have been shown controlling a ferromagnetic thermo-
plastic with thermal patterns and magnetic fields. This works opens up applications in tactile displays and object
manipulation. We highlight the capability of microwave and magnetic fields to pass through optically opaque
materials, making these manipulations suitable for operating in biological tissue or plastic containers.

Methods
Compound mixing.  The samples were prepared by solution casting a mixture of polycaprolactone (PCL,
Polydoh Materialix) with iron particles of 100µ m with 98% purity (Alquera). Dichloromethane (DCM) and
hexane (Sigma Aldrich) solvents were used to ensure good blending.
In this process, five samples (S10, S20, S30, S40 and S50) with different iron content in volume were pre-
pared inside a cubicle with an extractor hood and under normal conditions at room temperature. A beaker of
1L capacity was placed on a hotplate IKA C-MAGHS7 with a temperature controller IKA ETS-D5 and a digital
stirrer LaboLan OS40-S, equipped with a mixer paddle. First, the DCM solvent temperature is settled at 30 ◦ C
inside the beaker. The amount of solvent was ten times in volume the mass of polymer to be dissolved, e.g. 200
ml solvent for 22 g of PCL. Then, the polymer was added. The reaction was carried out at 30±2 ◦ C and stirred
for 2 h at a speed of 300 rpm. Once the polymer was totally dissolved, the iron powder was incorporated to the
solution and mixed for 1 h, increasing the mechanical stirring speed up to 500 rpm. After the iron particles were
completely dispersed, 100 mL of hexane was added to promote the composite precipitation and the solution
temperature was increased to 50±2 ◦ C in order to evaporate both solvents.
Once the mixture is homogeneous and the solvents have disappeared, the mixture can be removed and put
into a mould. For minimising the differences within the experiments, a volume around 21.34 cm 3 was settled for
each sample considering the mould capacity and materials density: PCL ( ρ = 1145 g/cm3 ) and iron ( ρ = 7874
g/cm3 ). These silicone moulds were used for creating 3D cylindrical shape samples. The 2D sheets were crafted
the same way, but instead of putting them in a mould, they were flattened with a stainless steel rolling pin on a
silicone mat. For the 1D filaments, the compound was shredded into pellets and introduced in an extruder (FelFil
Evo equipped with a 1.75 mm circular cross section nozzle) at 60 ◦ C and 6 mm/s of speed. Samples can be seen
in Supplementary Fig. 1 and the resulting weight of the volume proportions in Table 1.

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Figure 6.  (a) Heating with a GE 4405 PAR36 lamp of 12.8 V and 30 W focusing the light with a planoconvex
aspheric lens LAF6075. (b) Heating with a MMOBIEL Yihua 858D hot-air soldering station. (c) Heating with
Beurer IL21 infrared lamp. (d) Heating with a 3M 9000 AHKS overhead projector: using a mask and a focusing
planoconvex aspheric acrylic lens of 90 mm ∅ and F = 20 mm. (e) Heating with a Taurus W750MG microwave.
(f) Heating with a Vevor 3B 450 nm and 2500 mW blue laser. (g) Temperature evolution using different heat
sources over 60 s.

Thermal sources.  Different thermal sources were used during the experiments: a focused halogen lamp,
hot air gun, IR lamp, acetate masks projector, laser and microwave. They are shown in Fig. 6.

Thermal measurements.  A thermal camera RS PRO T-10 (RS Components) was used to measure the
temperature on the samples at different points. In the bulk thermal conductivity experiment, the samples were
heated on a hot-bed from an (Ender 3 PRO 3D printer) that was set in closed-loop at 50 ◦ C. In the point spread
thermal experiment, the focused halogen lamp (GE 4405 PAR36 30 W) was used to heat the middle point of the
surface of each sample. The focal light was set at a distance of 5cm from the tip of an aspheric acrylic lens (Knight
Optical LAF6075). The lamp was working at its nominal power.

Magnetic sources.  Different magnets were used for generating the magnetic fields that manipulated the
samples they can be seen in Supplementary Fig. 3. Their field was measured with a teslameter (WT10A). The
magnets were moved manually, with tripods or with linear stages.

Magnetic measurements.  For the magnetic force measurement, each sample was attached into a magnet
(Wukong 304 M8 neodymium N52) and an increasing downwards force was applied until the sample detached
from it. The magnet was hanged from a digital dinamometer (GPISEN 50 kg, 5 g error) as it is shown in the
Fig. 6g. The force was recorded as the maximum force needed to detach the magnet.

Data availability
Data generated or analysed for this research are included in the published article and its supplementary infor-
mation files.

Received: 10 September 2022; Accepted: 16 November 2022

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Acknowledgements
This research is funded by the EU Horizon 2020 research and innovation programme under grant agreement
No. 101017746 TOUCHLESS.

Author contributions
J.I., I.E., X.S. and I.G. conducted experiments. J.I. and A.M. wrote the paper. J.I. and I.E. recorded and edited
supplementary videos. J.I. and I.E. created the figures. J.I. and I.G. crafted the samples. A.M. ideated the research
and made the simulations. All the authors contributed by editing the manuscript.

Competing interests 
The authors declare no competing interests.

Additional information
Supplementary Information The online version contains supplementary material available at https://​doi.​org/​
10.​1038/​s41598-​022-​24543-5.
Correspondence and requests for materials should be addressed to A.M.
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