Roh et al.

Nano Convergence (2023) 10:20 Nano Convergence

https://doi.org/10.1186/s40580-023-00369-3

REVIEW Open Access

Applications of remote epitaxy and van der

Waals epitaxy
Ilpyo Roh1,4†, Seok Hyeon Goh2†, Yuan Meng1, Justin S. Kim3, Sangmoon Han1, Zhihao Xu3, Han Eol Lee2*,
Yeongin Kim5* and Sang‑Hoon Bae1,3*   

Abstract
Epitaxy technology produces high-quality material building blocks that underpin various fields of applications. How‑
ever, fundamental limitations exist for conventional epitaxy, such as the lattice matching constraints that have greatly
narrowed down the choices of available epitaxial material combinations. Recent emerging epitaxy techniques such
as remote and van der Waals epitaxy have shown exciting perspectives to overcome these limitations and provide
freestanding nanomembranes for massive novel applications. Here, we review the mechanism and fundamentals for
van der Waals and remote epitaxy to produce freestanding nanomembranes. Key benefits that are exclusive to these
two growth strategies are comprehensively summarized. A number of original applications have also been discussed,
highlighting the advantages of these freestanding films-based designs. Finally, we discuss the current limitations
with possible solutions and potential future directions towards nanomembranes-based advanced heterogeneous
integration.
Keywords Remote epitaxy, Van der Waals epitaxy, 2DLT, Heterogeneous integration, Freestanding membrane

1 Introduction induces periodic fluctuations in the surface potential

Epitaxy is a material deposition process producing and acts as a driving force for atomic nucleation. Strong
epilayers by copying crystallographic information of sub- chemical bonding is responsible for lattice alignment
strates. The dangling bond between the crystalline sub- in epitaxial growth, allowing the epilayer to mimic the
strate and the atom of the epitaxially formed material crystalline structure of the substrate. The epitaxial layer
is thus tightly bonded to the substrate with high bind-
ing energy. Due to this strong bonding, it is difficult to
Ilpyo Roh and Seok Hyeon Goh contributed equally to this article. separate the epitaxial layer from the growth substrate.
*Correspondence:
However, the demand for detaching the epitaxial layer
Han Eol Lee fields is increasing in various new applications. For exam-
[email protected] ple, the separated thin epitaxial layer, called freestand-
Yeongin Kim
[email protected]
ing nanomembranes, can be physically light and flexible
Sang‑Hoon Bae because of substantially reduced thickness and stiffness.
[email protected]
1
In addition, it is possible to achieve unprecedented per-
Mechanical Engineering & Materials Science, Washington University
in St. Louis, Saint Louis, MO 63105, USA
formance and multifunctional function by stacking the
2
Division of Advanced Materials Engineering, Jeonbuk National ultrathin films of different characteristics and functions
University, Jeonju 54896, South Korea
3
that have grown independently on different substrates.
The Institution of Materials Science & Engineering, Washington
University in St. Louis, Saint Louis, MO 63130, USA
These characteristics are vital for novel applications,
4
R&D CENTER, M.O.P Co., Ltd, Seoul 07281, South Korea including flexible-displays, bioelectronics, and the Inter-
5
Department of Electrical and Computer Engineering, University net of things (IoT) [1, 2].
of Cincinnati, Cincinnati, OH 45221, USA

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Roh et al. Nano Convergence (2023) 10:20 Page 2 of 17

To date, several methods such as chemical lift, opti- as their ionicity increases. Also, it is important to have
cal lift, and laser lift-off were developed to separate high thin 2D materials to utilize remote interaction through
quality epitaxial layers from the growth substrates [3, 4]. 2D materials because thick 2D materials screen potential
Chemical lift-off uses a sacrificial layer inserted between penetration coming from substrates [8]. Therefore, it is
the substrate and the epilayer. The sacrificial layer is important for successful remote epitaxy to induce uni-
removed selectively for obtaining a freestanding film. form field penetration through control of the number of
The higher the etching selectivity of the sacrificial layer, 2D materials [9–11].
the less damage to epitaxial layer is typically observed. Unlike conventional epitaxy, there is vdW bonding at
Laser lift-off uses the laser energy absorption difference the interface between the grown materials and substrates,
between the epitaxial layer and the substrate. For exam- allowing exfoliation of the grown materials. This looks
ple, in the GaN and SiC structures, the GaN epitaxial analogous to the mechanical exfoliation of spalling, but
layer can be exfoliated from the substrate because the it is capable of exactly determining the interface where
photon is mostly absorbed in a thin GaN interface layer. exfoliation happens. As 2D materials have the weakest
Mechanical lift-off is a technology using the cracks near interface, layer separation occurs at 2D materials. With
the edge. It can exfoliate epitaxial layer from substrate such feature, precise thickness control of freestanding
with crack propagation parallel to the surface. However, nanomembranes are achievable through it [12].
these processes include limitations such as few selection
of materials, surface damages from breaking strong bond 2.2 vdW epitaxy growth
and low throughput of layers [5, 6]. VdW epitaxy is the growth of the epitaxial layer on a
To overcome these limitations, remote and van der crystalline substrate, where the epilayer is held together
Waals (vdW) epitaxy technologies have been proposed as with the substrate by a weak vdW interaction [13, 14].
a growth method together with a new layer transfer tech- Since this weak vdW interaction does not have covalent
nique called 2D material-assisted layer transfer (2DLT) bonding in out-of-plan, the growth layer can be formed a
[7]. Massive researches have been reported based on crystallization regardless of the 2D material crystal struc-
this technique. Using 2DLT, the epitaxial layer is grown ture. In addition, since the coated 2D material can screen
on a substrate coated with vdW materials. Between the the electrostatic potential of the growth substrate: it can
epitaxial layer and vdW materials, there is only a weak suppress the strain caused by the lattice constant differ-
physical bond because of no strong covalent bonding in ence between the substrates and the grown materials, and
out-of-plane. Thus, the epitaxial layer can be easily sepa- the epitaxial layer can be grown regardless of whether the
rated from weak vdW bonds through the 2DLT. substrate is polar or non-polar [15–33]. However, this is
Here, we review recent progress in advanced epitaxy accompanied by disadvantages of reducing the quality of
technologies of remote and vdW epitaxy and their appli- grown films by inhibiting the nucleus generation neces-
cation based on the 2DLT. The unique advantages are dis- sary for the formation of crystal on 2D surface. Therefore,
cussed that can be obtained from these growth methods, to obtain a high quality vdW epilayer, 2D interlayer such
including universality, transferability, cost reduction, and as multi-layer graphene should fully screen the electro-
high crystal quality. In addition, representative applica- static potential of the substrate is required and finding
tions of electronic, optoelectronic, and electrochemical the optimized growth conditions that can quickly gener-
device developed based on these technologies are also ate nucleus on the surface is also important as well.
explored. Finally, we discuss the current limitations of the In the same way as remote epitaxy, vdW epitaxy adapts
two growth methods, as well as possible solutions and a growth structure in which vdW material is inserted
future directions towards heterogeneous integration. between the substrate and the grown materials, free-
standing nanomembranes can be obtained with the same
2 Advanced growth methods transfer method.
2.1 Remote epitaxy growth
Remote epitaxy is an exemplary material growth method 3 Unprecedented advantages of remote and vdW
to produce materials on 2D material-coated substrates epitaxy
using remote interaction coming from substrates [8]. The 3.1 Universality
magnitude of the remote interaction is determined by the Since remote epitaxy and vdW epitaxy can grow vari-
strength of the polarity of the substrate materials and the ous materials in 2D materials-coated substrates, the lim-
vdW gap distance. Therefore, materials having polarity ited selection of materials in the conventional growth
such as III-V, III-N, complex oxide, and halide- perovs- method can be overcome. The vdW epitaxy growth
kite have been explored. It is confirmed that the pene- of β-Ga2O3 film on graphene/SiC substrates has been
trated potential field of such polar materials gets stronger reported, where graphene is directly formed on the SiC
Roh et al. Nano Convergence (2023) 10:20 Page 3 of 17

using high temperature treatment process before grow- vdW epitaxy method. In this study, they investigated the
ing β-Ga2O3. The graphene was favorably influenced by growth behavior of Al atoms on ­O2-plasma-assisted pat-
lattice arrangements of SiC substate, and thus enabled terned graphene for improving epitaxial quality. By pat-
direct-epitaxy of β-Ga2O3 on the graphene. Also, the terning graphene with O­ 2 plasma, the adsorption barrier
β-Ga2O3 layer was spontaneously exfoliated at the inter- of Al atoms is greatly reduced and improve the growth
face of graphene owing to its low interfacial toughness by quality of the AlN buffer layer. Finally, the high-quality
controlling the energy release rate through electroplated and large-area GaN epitaxial layer with low dislocation
Ni layers as shown in Fig. 1a [34]. Moreover, Hao et al. density is obtained, and transfer and flexibility are suc-
grew the high-quality transferable GaN based on the cessfully achieved as shown in Fig. 1b [35]. For other

Fig. 1 a. Schematic illustration explaining the principle of the exfoliation of β-Ga2O3 from the graphene on SiC and photograph of the exfoliated
β-Ga2O3 nanomembrane; the inset indicates a flip of 180° for the nanomembrane [34], b. Photograph image of flexible GaN film transferred from
graphene/sapphire substrate [35], c. Schematic of various vdW oxide heteroepitaxy of ZnO, M ­ oO2, ­CoFe2O4, ­Fe3O4, ­PbZrTiO3, ­VO2 [22, 36–41], d.
Schematic views of remote epitaxy of III-V on graphene/III-V substrate and exfoliation of grown III-V layer, e. Photographs of single-crystalline
GaAs(001) exfoliated from graphene GaAs(001) substrate [42], f. Schematic illustration depicting fabrication procedures for flexible GaN-LED array
encapsulated with polyimide filler, g. Photograph of polyimide encapsulated GaN-LED exfoliated from substrate [43], h. Schematics depicting the
exfoliation of the heteroepitaxial ZnO microrods process using the thermal release tape technique, and corresponding result sample photographs
of ZnO microrods coated by PI [44]
Roh et al. Nano Convergence (2023) 10:20 Page 4 of 17

materials, various vdW oxide epitaxial layers have been and electrochemical with new stacked heterogeneous
studied. The most common oxide structure has been structure. To implement this, several lift-off technologies
demonstrated in the heterostructure with epitaxial rela- have been developed so far. Chemical lift-off is a method
tionships as shown in Fig. 1c [22, 36–41]. Since there of creating freestanding epitaxial films by inserting a sac-
is no strong chemical bonding between the layer and rificial layer that can be selectively etched in between the
the substrate, the quality of vdW oxide heteroepitaxy epitaxial layer and the substrate as shown in Fig. 2a. For
depends on the competition of surface energy and the example, for freestanding GaAs, AlGaAs can be etched
coherency of the symmetry between muscovite and epi- by hydrofluoric acid whereas InGaAs-based materials
taxial layer. Typically, three- or six-fold axis with the low- are resistant to hydrofluoric acid, allowing AlGaAs to be
est surface energy will be the orientation of epitaxial layer used as a sacrificial layer [45–51]. Laser lift-off separates
on muscovite. In most oxide epitaxial layers on musco- epitaxial layers from transparent substrates such as sap-
vite, the lattice constants and properties were shown to phire or SiC using high energy excimer lasers as shown
be close to bulk materials or single crystals. in Fig. 2b. For example, in substrate/GaN structure, a
For remote epitaxy, many recent research results have short-wavelength laser is used, which is absorbed by the
been reported for producing various high quality epi- GaN film, decomposing the substrate/GaN interface into
taxial films. Kim et al. recently published research results metallic Ga and N ­ 2 gas, which can then be heated above
on the successful growth of III-V (001) epitaxy on III-V the melting pint of Ga to separate the epilayer from the
(001) substrates using graphene [42]. For example, as substrate [52–54]. Mechanical spalling is a brute force
shown in Fig. 1(d, e), they demonstrated the feasibility method of creating thin films in micrometers-thick
of growing single-crystal GaAs (001) based monolayer range, where a metal stressor layer is used to initiate a
graphene overlayers on GaAs (001) substrates and exfo- crack running parallel to the substrate as shown in Fig. 2c
liating grown GaAs (001) from substrate. Furthermore, [55–63]. However, these techniques commonly takes
Hong et al. explained that the remote epitaxy of GaN a long time to remove the interlayers of the substrate
p-n homojunction microcrystal is demonstrated using and film, which limits throughput and harms mass pro-
metal–organic chemical vapor deposition (MOCVD) duction. In addition, when the epitaxial is mechanically
for fabricating transferable, flexible while light-emitting lifted, the roughness of the substrate becomes severe and
diodes as shown in Fig. 1f. Figure 1g shows that the GaN- there is a constraint in the reuse of the substrate.
LED microcrystal peeling off is possible with a weakly However, since the two-dimensional layer transfer
bond interface [43]. For other materials, the remote (2DLT) technology based on vdW and remote epitaxy
heteroepitaxy of ZnO microrods on the GaN substrate can easily exfoliate the 2D material between the substrate
across graphene layer via hydrothermal graphene has and the grown nanomembranes as shown in Fig. 2d, the
demonstrated [44]. Through density-functional theory transfer time of the membrane is reduced and the pris-
calculations, they found that charge transfer along the tine surface remains after exfoliation, [64, 65]. Thus,
z-direction in multilayer of graphene (MLG)/c-GaN can no wafer refurbishing processes such as chemical and
attract adatoms leading to remote heteroepitaxy. Based mechanical polishing is required.
on the calculation results, they conducted a remote epi-
taxy of ZnO microrods experiment using a three-layer 3.3 Cost reduction
MLG, and Fig. 1h shows related results. One significant advantage of the freestanding nanomem-
branes is their potential to enable wafer recycling [66].
3.2 Transferability One key stamping block for the widespread application
Since freestanding membranes have a unique vdW inter- of non-Si semiconductors like GaAs, GaN, SiC, etc. is the
face, they can allow heterogeneous integration of dissimi- expensive material cost arising from the high-cost sub-
lar materials. This attribute opens an exciting platform for strates. However, in most cases the substrate only serves
an unprecedented application of electron, photoelectron, as mechanical support, and only the top thin material
(See figure on next page.)
Fig. 2 a. Schematics of epitaxial lift-off techniques using a chemically etched sacrificial layer, b. An optically induced separation between the
epilayer and substrate, c. Brule-force mechanical spalling using a metal stressor layer, d. 2D material assisted layer transfer [64], e. Schematic
illustration explaining the 2DLT and recycling substrate, f. Atomic force microscopy (AFM) image of the surface of the GaN grown on the graphene
buffer layer. The RMS roughness is 0.18 nm, g. Photograph of the three-times-reused substrate and the exfoliated GaN epilayers [67], h. Schematic
of successive multiple membranes production by 2DLT and wafer recycling, i. Photographs of exfoliated membrane surface (top) and EBSD map
(bottom) [68], j. X-ray rocking curves of AlN grown on sapphire (black line) and plasma treated-graphene/sapphire substrates (red line), k. Atomically
resolved STEM image of the interface of AlN/graphene/sapphire [72], l. Strain-relaxation efficiency of InGaP grown on graphene/GaAs and on GaAs
[73], m. Schematic diagram of strain relaxation via the dislocation, the T indicates where a dislocation forma, and the schematic diagram below is
strain via spontaneous relaxation, n. Cross-sectional view of GaP grown on bare GaAs, o. Cross-sectional view of GaP grown on graphene/GaAs [58]
Roh et al. Nano Convergence (2023) 10:20 Page 5 of 17

Fig. 2 (See legend on previous page.)

layer functions as devices. The freestanding thin films of the top functional material layers from the 2D mate-
harvested from the remote epitaxy and vdW epitaxy can rial (generally graphene)-coated substrates as shown in
potentially enable wafer recycling after the exfoliation Fig. 2e [67]. The atomic force microscopy (AFM) image
Roh et al. Nano Convergence (2023) 10:20 Page 6 of 17

in Fig. 2f shows a smooth as a grown surface. Figure 2g energy required to displace the bonding at the interface
shows that 2D based growth technique enables reusing is weaker than that required to introduce a dislocation,
of the same substrate three times without any polishing the strain could be relaxed without introducing a dislo-
process. Moreover, in order to improve harvest epitaxial cation. In order to explain the theory more clearly, an
layers, the method of growing multiple epitaxial mem- experiment was conducted. Figure 2n, o show two TEM
branes method has been researched as shown in Fig. 2h cross-section images of GaP grown on GaAs without and
[68]. In this method, 2D materials are directly formed on with graphene interlayer respectively. The results show
substrates in epitaxy systems, which enables an advanced that there is a high-density dislocation with significant
remote epitaxy scheme comprised of multiple alternat- deformation patterns near the existing heteroepitaxial
ing layers of 2D materials and epitaxial layers that can be interface of GaP-GaAs. On the other hand, the disloca-
formed by a single epitaxy run. Figure 2i shows the meas- tion was significantly reduced in the heterogeneous epi-
urement data of the exfoliated surface by the 2DLT pro- taxial interface of the GaP-Gr-GaAs.
cess after multi-epithelial growth. Through this result, it
was confirmed that the GaN epitaxial layer has a smooth
surface shape without any damage during the exfoliation 4 Applications
of upper layer. Freestanding membrane produced by using remote and
vdW epitaxy growth methods can be integrated with
various other functional membranes. For example, free-
3.4 High crystal quality standing membrane can be transferred to heat sink
Applying an ultra-thin atomic layer between the epitax- substrate, which can improve the heat dissipation prop-
ial layer and substrate in the heteroepitaxy system is an erty. In addition, the integrated structure with other
important technology that can grow high crystal quality membranes that change physical properties according
films without dislocation in not only lattice matched but to chemical and physical reactions makes it possible to
also lattice mismatched conditions. In the vdW epitaxy realize the multifunctional devices that can be applied to
method, the single-crystal thin films can be grown by various areas.
effectively reducing the mismatch effect due to the weak
bonding between III-N and graphene and alleviating the
self-heating problem [12, 14, 68–71]. Liu et al. success- 4.1 Electronic application
fully grew single-crystal AlN by improving III-N nuclea- For electronic applications, vdW epitaxy and subsequent
tion on graphene using plasma-treated graphene [72]. transfer can be used to improve heat dissipation required
In this research, through DFT calculations, it was found by radiofrequency (RF) devices. AlGaN/GaN high-elec-
that pyrrolic nitrogen in graphene introduced by plasma tron-mobility transistors (HEMT), one kind of RF device,
treatment facilitates AlN nucleation and enables fast were transferred to a higher thermal conductivity than a
growth. Figure 2j shows that the (0002) full width at half growth substrate to suppress the self-heating effect and
maximum (FWHM) of the X-ray ω-scan (rocking curve) increase drain currents [15]. As shown in Fig. 3a, an
of the AlN epilayer is significantly reduced from 698.6 to AlGaN/GaN heterostructure was grown on AlN (nuclea-
315.5 arcsec with the assistance of graphene. Also, Fig. 2k tion layer)/h-BN/sapphire. An AlGaN/GaN HEMT with
shows STEM images of AlN/plasma treated graphene/ a Schottky Au/Ni gate electrode and ohmic Au/Ni/Al/
sapphire grown by vdW based on calculated results. The Ti source/drain electrodes were fabricated using photoli-
results show that single crystals of AlN were grown on thography and a lift-off process. The AlGaN/GaN HEMT
sapphire substrates without dislocations. device can be mechanically transferred from the sap-
In the remote epitaxy growth method, the research phire wafer using the h-BN as a release layer. After the
about the mechanism of relaxing misfit strain in heter- deposition of Ti/Au/In layers on the released AlGaN/
oepitaxial films that can enable effective lattice engineer- GaN HEMT, the HEMT/Ti/Au/In was bonded to a Cu
ing was reported [73]. Figure 2l shows the InGaP/bare plate using thermal fusion bonding. The AlGaN/GaN
GaAs and InGaP/Graphene/GaAs with 0.74% tensile HEMT that was not transferred showed a decrease in
strain for demonstrating graphene-based strain relaxa- drain current by 30% with increasing drain voltage above
tion. In these structures, the result shows that the relaxa- saturation voltage, which is attributed to the self-heating
tion gradually increases as the thickness of ­In0.4Ga0.6P effect. On the other hand, in the transferred AlGaN/
increases, and I­ n0.4Ga0.6P layer grown in graphene/GaAs GaN HEMT, the decrease in drain current was only 8%,
is particularly spontaneously relaxed. Furthermore, this as shown in Fig. 3b. Transfer from the sapphire to the
result means that as assumed in Fig. 2m, there is an copper plate mitigates self-heating effect because copper
alternative relaxation pathway that can be immediately has higher thermal conductivity than sapphire in Fig. 3c.
relaxed on the graphene surface. More specifically, if the Heterogeneous integrated structures with substrates with
Roh et al. Nano Convergence (2023) 10:20 Page 7 of 17

high heat dissipation efficiency can improve the perfor- (sacrificial metal layer)/(Si wafer) with epoxy adhe-
mance of RF and power devices. The reported electron sives. Subsequently, conventional cleanroom processes
mobility and sheet electron density of the 2D electron gas were utilized to make a stretchable surface acoustic
at the AlGaN/GaN interface was 1360 ­cm2V−1 ­s−1 and wave device made of the GaN film integrated with a
7.4 × ­1012 ­cm−2. stretchable antenna in Fig. 3g. A simulation of SAW
Flexible electronics are one of the main applications of generation was performed to analyze the performance
freestanding epitaxial films prepared by vdW epitaxy. For improvement of the device. The results show that the
flexible devices, the conductive bottom layer with a sin- electromechanical coupling coefficient ­K2 is negligible
gle crystallinity is desirable to epitaxially grow the active for substrate-bonded GaN films thinner than 300 nm
layer on top of the bottom electrode. Metallic ­MoO2 with as shown in Fig. 3h. Substrate binding alters the acous-
high crystallinity was grown on a flexible muscovite sub- tic mode and substantially reduces the displacement
strate [22]. The similar crystal structures of ­MoO2 and amplitude of acoustic oscillations. However, since the
muscovite lead to epitaxial growth even with the weak GaN layer in the proposed structure is de-clamped
vdW force between them. The resulting monoclinic with the substrate, the electromechanical coupling is
­MoO2 epitaxial layer on the muscovite could be used greatly improved by eliminating the coupling effect. In
not only as a bottom electrode but also as a base layer this SAW based chip-less wireless e-skin, an ultra-thin
for the heteroepitaxial growth of other oxide layers on GaN SAW sensor can cope with chips, circuit parts
top of the ­MoO2 layer. Figure 3d shows the sample flex- and sensors. They can also be incorporated into thin
ible ­MoO2/muscovite, which it can be bent without any patches of perforated polydimethylsiloxane (PDMS) to
observable cracks appearing in the system. Due to the remove perspiration and skin by-products, providing
weak bonding between the layers of muscovite, it can be conformability, long-term wearability and significantly
cleaved much thinner than the conventional oxide sub- lower power consumption compared to chip-based
strates. Furthermore, in order to characterize the charge e-skins.
carrier type and carrier concentration of the ­MoO2 films, Moreover, the heterogeneous integration of piezo-
temperature dependent Hall measurements were car- electric and magneto-strictive material led to magneto-
ried out. Figure 3e shows a typical result of the vertical electrical coupling mediated by mechanical strain [75,
resistance R versus the magnetic field, in the range from 76]. A Pb(Mg1/3Nb2/3)O3-PbTiO3 (PMN-PT)/ ­ SrRuO3
− 2 T to 2 T at 10 K. The positive slope indicates that (SRO) layers were epitaxially grown on a S­ rTiO3 (STO)
­MoO2 is p-type. The carrier concentration, n, reaches a substrate. The piezoelectric PMN-PT can be exfoli-
value of 1.9 × ­1022 ­cm−3 and the carrier concentration in ated from the SRO layer because of the weak bonding
this ­MoO2/muscovite system shows almost no tempera- between them. Separately, a magneto-strictive ­CoFe2O4
ture dependence. The calculated mobility of ­MoO2 is 0.53 (CFO) layer was deposited by remote-epitaxy on a STO
­cm2V−1 ­s−1 at 300 K and 0.97 c­ m2V−1 ­s−1 at 2 K, shown substrate. The PMN-PT was transferred to a Ti-coated
in Fig. 3f. polydimethylsiloxane (PDMS) substrate. A 7-nm Pt
Surface acoustic wave (SAW) devices can be also top electrode was deposited onto the PMN-PT layer,
enabled by piezoelectric films made from remote epi- and the CFO membranes was transferred to the top of
taxy [74]. Single-crystalline piezoelectric GaN film Pt/PMN-PT/Ti/PDMS as shown in Fig. 3i. Then, the
was grown on a 2D material/GaN/sapphire by remote device was measured to magnetic induction and elec-
epitaxy. The GaN film was peeled off using a Ni trical coupling effect with the PMN-PT device clamped
stressor and bonded to the (flexible polyimide film)/ on the substrate. The stand-alone CFO/PMN-PT

(See figure on next page.)

Fig. 3 a. Schematic views of process sequence for the transfer of an AlGaN/GaN HEMT from a sapphire substrate to a copper plate, b. ­Id-Vds
characteristics of AlGaN/GaN HEMTs before release from sapphire (blue line) and after transfer to a copper plate (red line), c. temperature map of
the samples, taken with IR camera Neo Therno 700 (up-left and -right show the off state of the unreleased and transferred devices, respectively,
down-left and -right show the on state oof the unreleased and transferred devices, respectively) [15], d. the flexibility of M­ oO2/muscovite
sample(left) and removal of ­MoO2 film from muscovite substrate, e. carrier concentration of ­MoO2 films do not show any obvious temperature
dependence, f. mobility in the ­MoO2 films do not show any obvious temperature dependence [22], g. Chip-less wireless e-skin based on surface
acoustic wave (SAW) devices made of GaN freestanding membranes, h. Calculated electromechanical coupling coefficient (­ K2) of GaN SAW devices
by the function of GaN thickness [74], i. The device structure of CFO/PMN-PT magnetoelectric coupling device. In the case of clamped device, the
substrate and the bottom electrode are STO and SRO, respectively. In the case of the freestanding device, the substrate and the bottom electrode
are PDMS and Ti, respectively, j. The voltage generated across the PMN-PT film in response to the magnetic field input [75], k. Schematic illustration
of the BTO film growth, exfoliation, and transfer process onto a flexible PI substrate, l. Illustration of the experimental configuration of the c-AFM
test, m. I-V curve of the Pt/BTO junction, n. Evolution of the current as a function of loading force, o. COMSOL FEM calculation with a tip-force model
of the BTO film under applied force 28nN(up) and 196nN(down). The colors of blue to red correspond to lower to higher strain values [77]
Roh et al. Nano Convergence (2023) 10:20 Page 8 of 17

Fig. 3 (See legend on previous page.)

device produces a much larger voltage(δVME) than that the coupling effect is significantly enhanced when
the clamped device (477 ­mVcm−1) with a magnetic cell both are freestanding in heterogeneous stature of CFO
coupling factor of 27675 ­mVcm−1. These results show and PMN-PT as shown in Fig. 3j.
Roh et al. Nano Convergence (2023) 10:20 Page 9 of 17

Other than flexible electronics, freestanding epitaxial a tetragonal phase. The high gauge factor of the flexoelec-
films can benefit flexoelectric, piezoelectric, and mul- tric BTO can be attributed to excellent flexoelectric prop-
tiferroic devices. Although only materials with non- erty increased by (1) boosted strain gradient because of
centrosymmetric crystals show piezoelectric effects, all de-clamping of BTO from the substrate, different Young’s
materials including centrosymmetric materials show modulus and Poisson’s ratio of the cubic phase as com-
flexoelectric properties. In contrast to piezoelectric pared to the tetragonal phase, and the reduced thickness;
materials in which uniform strain generate polarization, and (2) high dielectric constant raised by oxygen vacan-
flexoelectric materials generate polarization in response cies in BTO. This research shows that the remote epitaxy
to strain gradient. The strength of flexoelectric polariza- of BTO film grown by remote epitaxy has great potential
tion becomes stronger as the flexoelectric film becomes for functional devices in oxide/semiconductor heteroge-
a freestanding film and possesses smaller dimensions neous integrated structures [78, 79].
because of the increase in strain gradient. As an example,
a flexoelectric ­BaTiO3-δ (BTO) film with a cubic phase 4.2 Optoelectronic application
was remote-epitaxially grown on a graphene-covered The III-V/III-N compound semiconductors are repre-
Ge substrate [77]. In contrast to tetragonal BTO films, sentative materials for inorganic thin-film optoelectronic
the cubic BTO film did not show piezoelectric property devices including light-emitting diodes (LEDs), solar
at room temperature, which was confirmed by piezo- cells, and photodetectors. Recently, these materials have
response force microscopy (PFM) measurement. The been spotlighted to realize heterogeneous integration
BTO film was exfoliated by using a Ni stressor layer and devices since they can be applied to the vdWE and the RE
a thermal release tape and was transferred to a target with efficient exfoliation and transfer onto flexible sub-
substrate, such as Au/Cr/polyimide. Figure 3k shows the strates. The vdW growth of a high-quality epilayer could
measurement using conductive-AFM (c-AFM), where be realized by using selective nucleation of III-N semi-
the Pt tip of the c-AFM cantilever forms contact with the conductor materials on the 2D layer. The violet LED was
exfoliated and transferred 10 nm-thick BTO film on the fabricated via the vdW epitaxy since AlN was selectively
Au/Cr/SiO2/Si substrate. Figure 3l exhibits the typical and directly grown at the optimal nucleation sites [80].
I-V curve obtained from the Pt/BTO/Au stack, indicat- The center of the graphene ring was the best adsorption
ing a rectifying behavior with a turn-on voltage of about site, and an AlN composite nucleation layer was formed
− 2.4 V. This indicates the BTO is n-type semiconducting between the 2D material and GaN epilayer using time-
and forms a Schottky junction with the Pt electrode. Fig- distributed and constant-pressure (TDCP) growth. This
ure 3m insert illustrates the band structure of this hetero- method allowed the growth/transfer of high-quality and
structure. In Fig. 3n, here the applied AFM tip bias was superior brightness violet LEDs, showing light output
set to − 4.3 V and it can be observed that, as the load- power of 260.5 W at 560 mA as shown in Fig. 4a. Deep-
ing force increases from 28nN, to 84nN, to 140nN, and ultraviolet (DUV) GaN LEDs were efficiently produced
196nN, the current varies from ~ − 12 nA to − 1 nA. To by using quasi-vdW epitaxy with N ­ 2 plasma-induced AlN
evaluate the strain distribution of the exfoliated BTO nucleation, enabling the 50% reduction of the process
film, particularly under different applied forces 28nN speed [72]. The interlayer graphene between the mother
and 196nN, simulation (COMSOL) finite element analy- wafer and AlN/GaN layers reduced mechanical biaxial
sis was performed and the results were shown Fig. 3o, in stress and the dislocation density in the epilayer due to
which the blue region on the film surface represents the the weak vdW interaction. The developed DUV-LED
AFM tip. This simulation result shows that the gauge fac- exhibited good rectifying characteristic with 4.6 V turn-
tor of flexoelectric BTO with a cubic phase is 1127, which on voltage and light output power of ~ 1.7 mW with the
is 4 times larger than that of piezoelectric BTO film with peak wavelength of 280 nm as shown in Fig. 4b.

(See figure on next page.)

Fig. 4 a. Light output power curve of violet LED which was grown by the vdW epitaxy [80], b. EL spectra of the vdW epitaxial DUV-LED [72], c.
Optical image of flexible solar-blind photodetectors using β-Ga2O3 epilayer [34], d. UV light on/off cyclic tests of flexible ­Ga2O3 photodetector [81],
e. I-Vds characteristics of ­WS2 epilayer-based photodetector according to ­Vgs [82], f. Fabrication procedure of GaN microrod/micropyramid arrays by
using the vdW epitaxy [83], g. Cross-sectional high-resolution TEM image and SAED patterns of AlN thin-film grown on the graphene/NPSS [30],
h. Cross-sectional SEM image and red light-emitting images of the remote epitaxial AlGaAs LED [90], i. Schematic image of DUV-LED on the h-BN/
sapphire wafer. The inset image shows a magnified microscopic image of DUV-LED array, j. Normalized EL spectra of DUV-LED by various injection
currents [91], k. Fabrication procedure of the remote epitaxial microrod LED array, l. Optical image of microcrystal-based LEDs emitting white light.
The right inset displays a magnified photograph of microcrystal-based LEDs, composed of orange, yellow, green, blue, violet, and white-emitting
nanocrystals, m. I-V characteristic of flexible microrod LED during 1000 bending cycles [101], n. Cross-sectional TEM image of the remote epitaxial
perovskite thin-film on a polar NaCl wafer. The inset presents FFT patterns of the C ­ PbBr3 film, o. Steady-state PL curve of the ­CsPbBr3 flakes on the
NaCl wafer and the graphene/NaCl substrate. [102]
Roh et al. Nano Convergence (2023) 10:20 Page 10 of 17

Fig. 4 (See legend on previous page.)

Oxide nanomembranes have been also considered as by the vdW epitaxy, and transferred to flexible substrates
promising materials for achieving 3D hetero-integrated for demonstrating the practical optoelectronic applica-
optoelectronic systems. The oxide thin-films were grown tions [34, 81]. A flexible solar-blind photodetector was
Roh et al. Nano Convergence (2023) 10:20 Page 11 of 17

realized by using a large-scale β-Ga2O3 film which was GaN microstructure-based LEDs monolithically emit-
grown by the vdW epitaxy on a compressive-strained ted blue (wavelength: 505.3 nm) and green light (wave-
epitaxial graphene as shown in Fig. 4c. The graphene length: 580.3 nm) according to the microstructures. This
grown along the SiC lattice was utilized as a buffer layer multicolor irradiation of the developed LED was attrib-
of the vdW epitaxy, enabling the successful β-Ga2O3 uted to the quantum-confined Stark effect from the dif-
nanomembrane growth. The oxide layer was spontane- ferent polarity of microrod and micropyramid LEDs. In
ously delaminated by the Ni stressor-based interface vdW epitaxy of AlN thin-films on the graphene, nano-
energy modulation, and fabricated to the vertical-struc- patterned sapphire substrate (NPSS) could assist to accel-
tured flexible photodetector. The flexible device displayed erate the material coalescence, efficiently minimizing the
excellent photosensitivity of 151.1 A/W at a wavelength growth time and the process cost [30]. Figure 4g depicts a
of 250 nm due to the wide band gap (~ 4.9 eV) of the high-resolution TEM (HRTEM) image and selected area
β-Ga2O3 nanomembrane. The vdW epitaxy of β-Ga2O3 diffraction (SAED) patterns of the AlN film grown on
thin-film could be applied to the mica substrate as well NPSS. The graphene interlayer on NPSS enabled reduc-
as the structure of 2D material/mother substrate because tion in Al migration barrier, the dislocation density, and
the mica wafer had a stacked structure of 2D-like thin the concentrated mechanical strain in the AlN epilayer,
framework layers [81]. The β-Ga2O3 thin-film grown on enhancing the AlN film quality. Following this research,
the mica was easily exfoliated by mechanical stress from vdW epitaxial membranes such as compound semicon-
a metal/adhesive tape-structured film, which could be ductors, oxides, TMDs, and microstructured III-N have
accomplished by intentional destruction of weak vdW been applied to various flexible functional optoelectronic
bindings between the mica layers. This exfoliation pro- devices.
cess was universally utilized for ­Ga2O3 films regardless of Recently, remote epitaxy has proven significant advan-
their material phase, film thickness and device-annealing tages, including the facile transferability of the vdW
temperature. The exfoliated ­Ga2O3 film had an excellent epitaxy and the capability to produce freestanding sin-
crystallinity due to the high-quality surface property of gle-crystalline nanomembranes. For instance, III-V thin-
the mica wafer, presenting self-powered UV detecting films produced from remote epitaxy can be handled by
performance of 17 mA/W at 0 V bias and 250 nm illumi- 2DLT to realize diverse photonic devices [7, 42, 88–94]
nation, as shown in Fig. 4d. for photonic integrated circuits and exploring nanopho-
Furthermore, the vdW epitaxy was adapted to form tonic physics [95–100]. Figure 4h displays the cross-
transition-metal dichalcogenides (TMDs) for acquiring sectional SEM image and the light-emitting images of
high-performance flexible photodetectors. Graphene- flexible AlGaAs LED [90]. Beside the LEDs with visible
WS2 (Gr-WS2) heterojunction was realized by the non- light (red, green and blue light), DUV AlGaN LED with
transfer method of a remote-catalyzed CVD, tungsten a 281 nm wavelength was realized by the remote epitaxy,
oxide deposition, and sulfurization by a plasma-enhanced as shown in Fig. 4i [91]. The AlN and DUV LED epilay-
CVD in successive processes [82]. The developed Gr-WS2 ers were directly grown by the MOPVE method onto the
heterojunction was conjugated to photodetectors by high-quality h-BN layer on the c-plane sapphire wafer.
making Al/AlOx top gate, and Cr/Au-based source/drain According to TEM analyses, the grown AlN layer had a
contacts. The device was easily transferred to flexible high crystal quality on 2.9 nm-thick h-BN, showing the
PET film, maintaining its optoelectrical properties of 4.0 wurtzite structure with (0001) c-axis orientation. The
A/W photoresponsivity, and fast ON/OFF switching as flexible tape-attached AlN layer was easily delaminated
shown in Fig. 4e. between h-BN layers owing to the weak adhesion force.
The vdW epitaxy could be applied not only in 2D-like The EL peak of DUV LEDs on the AlN/h-BN/sapphire
thin-films but also in micro structured III-N compound was stably maintained though the increasing injection
semiconductors [20, 21, 30, 34, 83–87]. Figure 4f depicts current from 5 to 40 mA as shown in Fig. 4j.
a schematic procedure of the ZnO nanorod template for- Remote heteroepitaxy has also been applied to low-
mation for realizing GaN microrod and pyramid arrays dimensional semiconductor materials such as nanowires
[83]. The ZnO nanorods were selectively grown through and microrods for solving the defect issue and the con-
the patterned ­SiO2 growth mask on the transferred gra- centrated strain of the epitaxially grown thin-film mate-
phene/SiO2/Si substrate, and the GaN LED layers were rials [43, 70]. As displayed in Fig. 4k, III-N compound
formed through heteroepitaxy on ZnO in sequence. semiconductor-based microrod LEDs were heterogene-
After metallization and passivation of the microstruc- ously formed through the graphene layer on the c-plane
ture GaN LEDs, heterogeneous integrated devices were sapphire substrate [101]. The microrod LED with a p–n
fabricated by wet etching the bottom ­ SiO2 layer and junction of core/shell structure was completely pas-
transferring it onto a heat shrink substrate. The flexible sivated with polyimide and transferred to a flexible Cu
Roh et al. Nano Convergence (2023) 10:20 Page 12 of 17

plate to fabricate a flexible heterogeneous integrated thin film has chemical stability and efficient light absorp-
LED. The flexible heterogeneous integrated LEDs main- tion properties in an aqueous environment. Therefore,
tained their optical and electrical performances with the high-quality vdW epitaxy PEC ­ (Fe2O3/ZnO/Mica)
excellent mechanical durability due to the fully-embed- structure significantly improves the photocurrent den-
ded device structure in the polymer passivation layer. sity in the visible light region compared to pure ZnO and
Furthermore, as an advantage of the flexible heterogene- ­Fe2O3 layers as shown in Fig. 5c. This figure presents the
ous integrated LED, the device was freely cuttable by a typical linear sweep I–V curves for pure ZnO, ­Fe2O3,
normal scissor for attaching onto various versatile curved and ­Fe2O3/ZnO electrodes under visible light irradiation
and conjugated surfaces. Although the flexible device (λ > 400 nm). It can be observed that the PEC activity of
showed white color by the naked eyes, the individual the ­Fe2O3/ZnO heterostructure (98 µA) is much higher
microcrystals emitted different colors of white, orange, than that of pure ­Fe2O3 (24 µA) and ZnO (15 µA) films.
yellow, green, blue, and violet in the magnified micro- For other applications, ultra-thin AlN grown on vdW
scopic images as shown in Fig. 4l. According to EL and using MBE equipment has improved electronic proper-
PL analyses, various-colored light came from deep-level ties as well as structural stability, which has expanded
states in the grown materials, which were closely related the application range [115–119]. The bond between the
with Si doping level and amount of gallium vacancy. closest Al and N atoms in AlN is formed by a bond com-
Moreover, the heterogeneous integrated LED exhib- bination of Al-pz and N-pz orbitals. Electrons are trans-
ited excellent opto-electrical properties in a thermal ferred from Al to N due to the negative charge difference
shock test (temperature range from − 40 to 100 ℃) and between Al and N atoms. Therefore, charge transfer from
mechanical fatigue tests with 1000 bending/unbending Al to N dominates several properties of ultrathin AlN,
cycles as shown in Fig. 4m. including the opening of the band gap. In addition, the
The modulation of the dislocation density in a hal- Al-N bond of AlN has a dipole moment, which also plays
ide perovskite thin-film was theoretically interpreted by an important role in the adsorption of gas molecules.
using density functional theory (DFT) and molecular- These features can be useful for sensor applications [93].
dynamics (MD) simulations, and experimentally con- Figure 5d shows four different adsorption sites on the
firmed by TEM analyses [102]. Based on the simulations, AlN surface. Gas molecules are adsorbed on this AlN
the electrostatic potential from NaCl and ­CaF2 polar sub- surface to accept or donate electrons. Figure 5e explains
strate was calculated by the DFT. Figure 4n depicts the the charge density difference when gas molecules are
STEM image and fast Fourier transform (FFT) pattern adsorbed on the surface of AlN [120]. According to the
of the remote epitaxial ­CsPbBr3 with an orthorhombic calculation results, H­ 2 adsorption causes n-type doping
lattice structure. The C ­ sPbBr3 thin-film showed excel- of AlN NSs, while molecules such as C ­ O2, CO, ­O2 and
lent crystallinity with well-indexed diffraction patterns NO are acceptors. That is, it makes AlN p-type due to
on the graphene/amorphous NaCl substrate. The kinetic electron charge transfer to gas molecules. This changes
mechanism of the remote epitaxy including thin-film the conductivity of AlN, and by measuring the degree of
growth, dislocation regulation and strain relaxation was change, gas molecules can be analyzed.
interpreted by MD simulation. The optical property and Moreover, SAW sensors can be applied to many fields
the effective carrier lifetime were investigated in ­CsPbBr3 by using surface acoustic wave deformation [121–134].
films grown by ionic and remote epitaxy. The perovskite Figure 5f shows a heterogeneous integrated structure of
film by the remote epitaxy exhibited 3 times higher PL ion-selective membrane (ISM) on flexible GaN grown by
intensity and 4 times longer effective lifetime due to the remote epitaxy [74, 93]. The sensor can monitor the con-
modulation of the dislocation density as shown in Fig. 4o. centration of ions in sweat, which can serve as an indi-
cator for conditions such as hyponatremia, kidney failure
4.3 Electrochemical application and high blood pressure. When specific ions are trapped
For photoelectrochemical (PEC) applications, a hetero- in the ISM of the heterogeneous integrated sensor, the
geneously integrated structure of necessary materials viscosity and mass of the membrane change, shifting the
can simultaneously improve high photocatalytic proper- resonance peak of the SAW sensor, and this movement
ties and excellent electron mobility [103–113]. Figure 5a can be used to detect variation in the ion concentra-
shows the heterostructure of F
­ e2O3/ZnO on a mica sub- tion of the surrounding fluid. Figure 5g, h illustrates the
strate with high optical transparency and thermal sta- results of in vitro wireless detection of ­Na+ ions using a
bility [114]. Based on TEM results, high-quality oxide ­Na+ ISM-coated GaN SAW device on e-skin. Continu-
heteroepitaxy of ­Fe2O3/ZnO can be fabricated on flexible ous recordings, indicate clear and consistent response
mica substrate as shown in Fig. 5b. In this structure, the and recovery of the output signal, collected by exposing
ZnO thin film has high electron mobility, and the F ­ e2O3 the e-skin to aqueous NaCl solutions containing varying
Roh et al. Nano Convergence (2023) 10:20 Page 13 of 17

Fig. 5 a. Structural schematic of the ­Fe2O3/ZnO/mica heteroepitaxy, b. Cross-sectional TEM image of the ZnO/mica and F­ e2O3/ZnO interface, c.
Linear-sweep voltammograms of pure ­Fe2O3, ZnO, and the F­ e2O3/ZnO electrodes with visible-light illumination and the inset photograph of flexible
­Fe2O3/ZnO/mica [114], d. The atomic structure of monolayer AlN and four possible adsorption sites, e. Charge density difference plots for C
­ O2/AlN,
­H2/AlN, CO/AlN, ­O2/AlN, NO/AlN [120], f. Photograph of an e-skin attached on the back of hand (top) and Schematic illustrations and wireless ion
sensors based on GaN SAW device coated with ­Na+ ion–selective membranes, g. Resonant frequency shift in the wireless signals obtained from a
GaN SAW ion sensor in response to changes in ­Na+ ion concentration, h. Continuous wireless recordings collected from a SAW ion sensor during a
series of alternating injections of 0.86 mM NaCl solution and distilled water over the e-skin [74]
Roh et al. Nano Convergence (2023) 10:20 Page 14 of 17

concentrations of ­Na+ ions. The result shows that the the high production cost. This problem can be solved by
detection limit of 0.86 mM represents a small value com- layer transfer technology, and advanced growth method
pared with the biologically relevant range of > 10 mM in of remote and vdW epitaxy also suggest a new type of
sweat, indicating the high sensitivity of the GaN SAW ion layer transfer technology, 2DLT. The 2DLT transfer tech-
sensor. nology together with these growth methods can rapidly
release high-quality growth materials and reuse expen-
5 Challenge sive substrates, effectively reducing production costs.
Remote and vdW epitaxy have several issues in apply- This provides an opportunity to mass-produce high-per-
ing 2D template-based growth technology to practical formance devices essential in a ubiquitous environment
technology despite the extraordinary potential and con- at low cost. Moreover, these technologies enable stacking
siderable progress. As the vdW surface does not have a multiple freestanding materials on a single host substrate.
dangling bonds out-of-plane, there is no orbital sharing The possibility of integrating heterogeneous materials
source during growing materials. Thus, the degree of allows for implementation of multifunctional devices that
supersaturation is extremely low compared to the cova- could not be implemented in one device. In addition, new
lent terminated surface, leading to high critical Gibbs heterogeneous structures provide a platform to discover
free energy. Because of such features, finding optimal new physical coupling phenomena that have not been
growth conditions for single crystalline growth is much realized. We believe that these opportunities could pro-
more challenging. Of course, in remote epitaxy, remote vide a solution to current technical challenges as well as a
interaction helps periodic nucleation on vdW surface, guide to innovative technology in the future.
but it is still challenging. Also, for the remote epitaxy,
it is important to preserve clean interface between 2D Author contributions
materials and substrates and have uniformly thick 2D All authors read and approved the final manuscript.
materials on substrates. There are two methods to form
Funding
2D materials on substrates; (i) direct grow on substrates This work in JBNU was supported by the National Research Foundation of
and (ii) transfer on substrates. However, direct growth Korea (NRF) grants funded by the Ministry of Science, ICT and Future Planning
on substrate is challenging because of difficulty in kinetic (MSIT) (NRF-2022R1F1A1066064, and 2022R1A4A3033320).

control of 2D materials. This causes variation of thickness Data availability

and random orientation, making it difficult to obtain uni- The review is based on the published data and sources of data upon which
form 2D materials on substrates. In the transfer process, conclusions have been drawn can be found in the reference list.

process defects such as wrinkles, holes and residues are

always involved. Such defects hinder from having high Declarations
quality epitaxial layers. They can interfere with remote Competing interests
interaction, disrupting atomic guidance. Also, defective The authors declare that they have no competing interests.
sites generate covalent bonds at the interface between
grown materials and substrates, blocking the 2DLT pro- Received: 7 February 2023 Accepted: 9 April 2023
cess. Therefore, to overcome these limitations, a thor-
ough investigation of all kinetic parameters that affect
the growth process is necessary. Moreover, the transfer
process conditions that minimize stress on 2D materials References
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