Research Article

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Ultrathin, Flexible, and Transparent Oxide Thin-Film

Transistors by Delamination and Transfer Methods
for Deformable Displays
Jong Beom Ko, Seung Hee Lee, Tae-Ik Lee, Sangmin Lee, Jingyu Kim, Hyeok Kim,
Taek-Soo Kim, and Sang-Hee Ko Park*

applications such as in wearable devices,

The attachment of display devices to various objects has attracted much glasses of transportation and buildings,
attention due to their ability to present visual information to people in different and mirrors.[1–3] The transparent organic
environments. Such devices should be ultrathin to ensure complete coverage light-emitting diodes (OLEDs) and micro-
light emitting diodes (micro-LEDs) are
when attached to various objects, making them a critical technology for the
the optimal candidates among the various
development of rollable and stretchable displays. In this study, the fabrication display devices for the aforementioned
of high-performance ultrathin oxide thin-film transistors (TFTs) on a 5 µm-thick applications. This is attributed to the
polyethylene terephthalate substrate is demonstrated by the method of outstanding performances and relatively
delamination and transfer. Molybdenum oxide functions as an exfoliation layer, high power efficiencies of the OLEDs and
and the ultrathin devices exhibit full coverage on various objects with complex micro LEDs.[4,5] Furthermore, backplane
devices play a critical role in the develop-
surface profiles such as contact lens, fabric, and human skin. It is notable that ment of next-generation displays.
the TFT device exhibits a high optical transparency of greater than 81% and a Thin-film transistors (TFTs) are utilized
reasonable electrical performance with a high mobility of 37 cm2 V−1 s−1. Since as the backplane devices for active matrix
the oxide TFTs are fabricated without temperature limitations, the devices show (AM) liquid-crystal displays, AM organic
reliable electrical performances under gate and illumination stresses. The flexible light-emitting diode (AMOLED) displays,
AM-LEDs, and quantum-dot LEDs. TFTs
devices also exhibit excellent transfer characteristics in the bending state,
with amorphous oxide semiconductors are
regardless of the bending radius and direction, as well as a high mechanical suitable candidates for such applications
durability of over 10 000 bending cycles with the bending radius of 3 mm. owing to their multiple advantages such as
ease of fabrication, high electron mobility,
high electrical stability, and uniformity
1. Introduction over a large area.[6,7] Therefore, it is necessary to develop flexible
and transparent oxide TFTs that exhibit outstanding electrical
Deformable such as multi-foldable, rollable, and stretchable dis- performances. Furthermore, it is essential to design ultrathin
plays have attracted significant attention owing to their diverse display devices to ensure their complete coverage on and attach-
ment to various objects including stretchable substrates.
A typical fabrication method for flexible oxide TFTs includes
Dr. J. B. Ko, S. H. Lee, J. Kim, Prof. S.-H. K. Park a direct formation of film on a plastic substrate by a vapor dep-
Department of Materials Science and Engineering
Korea Advanced Institute of Science and Technology (KAIST)
osition, solution spinning, or bar coating, followed by photo-
291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea patterning.[8–10] However, most of the transparent plastic films,
E-mail: [email protected] including polyethylene terephthalate (PET) exhibit a high coef-
Dr. T.-I. Lee ficient of thermal expansion and a low glass transition tem-
Joining R&D Group perature (Tg).[11] These characteristics hinder the optimization
Korea Institute of Industrial Technology (KITECH) of the electrical performance of the oxide thin films that can be
156 Gaetbeol-ro, Yeonsu-gu, Incheon 21999, Republic of Korea
achieved by post-annealing at high temperatures. Furthermore,
Dr. S. Lee, Prof. T.-S. Kim
Department of Mechanical Engineering they also prevent the high-density integration of devices. To
Korea Advanced Institute of Science and Technology (KAIST) address these drawbacks, extensive research has been conducted
291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea on the application of heat-resistant plastic films like polyimide as
H. Kim flexible substrates.[12–14] However, these films exhibit a low optical
R&D Center transparency owing to their yellowish appearance. Although the
DAVO C&M
215 Amsogogae-ro, Yan-gam myeon, Hwaseong-Si, Gyeonggi-do 18635,
colorless polyimide can be processed at 300 °C as a substrate for
Republic of Korea oxide TFTs, the thick thickness (>10 µm) of such devices prevents
their applications to substrates with diverse surface profiles.
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/admt.202100431. To alleviate these issues, ultrathin flexible devices were
prepared by a technique involving delamination and transfer,
DOI: 10.1002/admt.202100431 where the TFT arrays were delaminated from a rigid substrate

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and transferred to various substrates with different surface reactive gas ratios. The results of the analysis are presented
profiles. Several groups have delaminated TFTs from rigid in Figure 1a. When molybdenum oxide was initially depos-
substrates via the chemical etching of the sacrificial layer to ited with a reactive gas ratio of 6:4 (Ar:O2), the XPS results
develop flexible optoelectronic devices, field-effect transistor, showed a dominant Mo4+ peak that corresponded to the com-
and other devices.[15–17] However, the chemical etching of position of molybdenum dioxide (MoO2). Therefore, this reac-
the sacrificial layer is a time-consuming process that limits tive gas ratio was not suitable for the deposition of the exfo-
the manufacturing of large sized flexible devices.[18,19] To over- liation layer. When molybdenum oxides were deposited with a
come this drawback, extensive research has been conducted on ­reactive gas ratio of 5:5 and 3:7 (Ar:O2), the XPS results showed
the delamination of devices using a physical force. Further- the presence of a dominant Mo6+ peak that corresponded
more, the successful fabrication of thin-film solar cells with to the composition of MoO3. A scrutiny of the Mo peaks
flexible substrates has been realized by crack or water-assisted revealed the presence of a relatively high concentration of
debonding.[20,21] Mo5+ in the film that was deposited with a reactive gas ratio
It has been reported that the delamination of films by the of 5:5 (Ar:O2). Therefore, a relatively low portion of oxygen in
debonding between two adjacent layers is accelerated under molybdenum oxide was obtained from the MoOx film that was
a corrosive environment.[22] In this study, we utilized water- deposited with the reactive gas ratio of 5:5 (Ar:O2). The atomic
soluble molybdenum oxide[23] as the exfoliation layer. This concentrations (in percentage) of molybdenum and oxygen in
allowed the device to be delaminated from the substrate owing the deposited molybdenum oxide films were determined from
to the reaction with the H2O in air at the crack of the interlayer the area of the Mo 3d and the O 1s peak, respectively, and the
region. The oxide TFTs were fabricated on a molybdenum oxide results are presented in Figure S1, Supporting Information. The
deposited on the glass substrate by the conventional process for molybdenum oxide film that was deposited with a reactive gas
fabricating display devices. The fabricated TFTs were subjected ratio of 6:4 (Ar:O2) contained a relatively low amount of oxygen.
to post-annealing; subsequently, they were detached from the The atomic concentration of oxygen in the molybdenum oxide
substrate using a physical force and transferred to the flexible, film increased with the increase in the proportion of oxygen in
transparent 5 µm-thick PET substrates. Since the oxide TFTs the reactive gas. The composition of the molybdenum oxide
were fabricated on a glass substrate, they could be processed at film that was deposited with a reactive gas ratio of 3:7 (Ar:O2)
high temperatures. This facilitated the optimization of the elec- was approximately identical to that of MoO3.
trical characteristics of the devices. The flexible and transparent The reactivity of the deposited molybdenum oxide with H2O
devices were attached to the objects with complex curvilinear was investigated by determining the etching rate in water. The
surfaces such as artificial leather, human skin, and contact lens. etching rates in water for the molybdenum oxide thin films that
The ultra-thin devices retained their outstanding electrical per- were deposited with a reactive gas ratio of 5:5 and 3:7 (Ar:O2)
formance in the bending state, despite the application of a high were compared. The analysis revealed that the etching rate in
bending stress. water varied significantly depending on the composition of
molybdenum oxide (Figure 1b). The molybdenum oxide film
deposited with a reactive gas ratio of 3:7 (Ar:O2) exhibited a
2. Results and Discussions higher solubility in water (26.2 nm s–1) as compared to that of
the film deposited with a reactive gas ratio of 5:5 (Ar:O2) (1.4 nm
The deposition of a suitable exfoliation layer is necessary to s–1). Furthermore, a research group led by Moon indicated that
delaminate the oxide TFTs from the rigid substrate. This study the water solubility of amorphous MoO3 was higher than that of
demonstrated the utilization of molybdenum trioxide (MoO3) the crystalline MoO3 owing to the intrinsic structural disorder
as the exfoliation layer because MoO3 can react with water to and the presence of defects.[23] The absence of noticeable sharp
form molybdic acid according to the following reaction:[24] peaks in the X-ray diffraction (XRD) pattern (Figure 1c) con-
firmed the amorphous nature of the molybdenum oxide film
MoO3 ( s ) + H2O (l ) → H2MoO4 ( aq ) (1) deposited by reactive sputtering. As a result, it is reasonable to
assume that the molybdenum oxide film deposited by reactive
Humid air acts as a corrosive environment for MoO3 owing sputtering reported here is highly soluble in water. Therefore,
to the water solubility of MoO3. This promotes the occur- the molybdenum oxide film deposited with a reactive gas ratio
rence of debonding in humid air. The environment-assisted of 3:7 (Ar:O2) eased the delamination by reacting with the H2O
debonding reaction is also facilitated by the formation of an in air, thereby inducing the environment-assisted debonding.
OH terminated fracture according to Equation (1). MoO3 The surface profile of the film was closely related to the
exhibits a higher reactivity with water than that exhibited by adhesion energy.[25] The surface area of the films increased with
other molybdenum oxides with different compositions. There- the increase in the roughness of the films. As a result, the con-
fore, an exfoliation layer comprising MoO3 was deposited by tact area between the layers increased, resulting in increased
reactive sputtering with a molybdenum (Mo) target in this adhesion energy. The surface profile of the molybdenum oxide
study. To regulate the chemical composition, the molybdenum layer was investigated by atomic force microscopy (AFM) and
oxide layer was separately deposited using a reactive gas mix- is presented in Figure 1d. The image revealed a smooth surface
ture with different ratios of argon (Ar) and oxygen (O2). with a root mean square roughness of 0.24 nm. Therefore, the
X-ray photoelectron spectroscopy (XPS) was performed to molybdenum oxide layer was suitable for use as the exfoliation
determine the chemical composition of the Mo peaks for the layer. In here, we adopted the 100 nm thick of molybdenum
molybdenum oxide films that were deposited with various oxide as the exfoliation layer.

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Figure 1. a) XPS Mo 3d peaks of the molybdenum oxide layers that are deposited with various reactive gas ratios. b) The thicknesses of the molybdenum
oxide etched in water depending on the reactive gas ratios. c) XRD pattern for the molybdenum oxide film on the glass substrate. d) Surface profile of
the molybdenum oxide layer, as determined by AFM.

Figure 2a shows a schematic of the process of transferring optical microscopy (OM) images of the flexible devices (Figure 2c)
the oxide TFT from the rigid glass substrate to the flexible and showed that the oxide TFTs were delaminated and transferred
transparent PET substrate. Prior to the fabrication of the oxide to the PET substrate without any noticeable damage generated
TFTs, the molybdenum oxide layer was deposited on the glass by cracking and wrinkling. The 5 µm-thick flexible devices uni-
substrate by reactive sputtering to form the exfoliation layer formly covered and attachment to objects with simple surface
(thickness = 100 nm). Subsequently, barrier layers comprising profiles such as glasses (Figure 2d) and contact lenses (Figure 2e),
180 nm-thick silicon nitride (Si3N4) as the bottom layer and objects with complex surface profiles such as clothes (Figure 2f),
20 nm-thick aluminum oxide (Al2O3) as the top layer were depos- and biological tissues such as human skin (Figure 2g) without
ited to prevent the contaminant-induced deterioration in the elec- wrinkling or the presence of delaminated regions when visually
trical characteristics of the TFTs. The oxide TFTs were fabricated identified. When the fabricated flexible devices in this study were
on the barrier layers using a vacuum-based process at a tempera- attached to different objects, they were not easily detected owing
ture below 350 °C. The processes for the fabrication of the oxide to their ultrathin and transparent nature.
TFTs are illustrated in Figure S2, Supporting Information. The To understand the mechanism of the easy delamination of
carrier film was spin casted on the samples and the oxide TFTs the oxide TFTs, the interface at the delamination region was
were delaminated from the rigid substrate by applying a physical investigated by high-resolution transmission electron micros-
force after the completion of the fabrication and post-annealing. copy (HRTEM). The debonding could occur at the following
The layers of molybdenum oxide and the inorganic barrier (Si3N4) interfaces: 1) between the barrier layer and the molybdenum
were easily separated at the interface by an applied physical force. oxide layer, 2) inside the molybdenum oxide layer, and 3)
The detached device, including the adhesive layer, was transferred between the molybdenum oxide layer and the glass substrate.
to the 5 µm-thick PET substrate, and the carrier film was removed The HRTEM image of the boundary between the delaminated
to open the electrode pad of the TFT device. Figure 2b shows region and the remaining area of the device was investigated to
the transferred oxide TFT on the 5 µm-thick PET substrate. The confirm the delamination surface. The analysis of the HRTEM

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Figure 2. a) Schematic illustration of the process of delamination and transfer. b) The transparent and flexible oxide TFT that is delaminated from the
rigid substrate and transferred to the 5 µm-thick PET substrate. The inset shows the picking of the flexible devices with tweezer. c) The magnified OM
image of the oxide TFT on the PET substrate. The inset indicates the magnified single-oxide TFT. A photograph of the flexible device that is attached
to the d) curved glass, e) contact lens, f) chest region of clothes, and g) back of the hand. The insets in each figure show the flexible devices reflecting
the lamp light.

image of the delaminated region (Figure 3a) indicated the delaminated region (Figure S3, Supporting Information).
removal of the oxide TFT with the silicon nitride barrier layer Therefore, the oxide TFTs were delaminated from the molyb-
during delamination; however, the molybdenum oxide layer denum oxide layer without leaving any residue.
remained intact. Therefore, it was confirmed that delamina- The HRTEM image confirmed the occurrence of debonding
tion occurred at the interface between the silicon nitride bar- between the silicon nitride and the molybdenum oxide layers.
rier layer and the molybdenum oxide layer. Furthermore, the Therefore, the adhesion energy between the two layers was
elemental mapping of molybdenum and silicon by energy- measured by the double cantilever beam method. The schematic
dispersive spectrometry revealed the absence of silicon at the of the double cantilever beam (DCB) specimen is presented in

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Figure 3. a) Cross-sectional TEM image of the oxide TFTs that are fabricated on the molybdenum oxide layer, including the delaminated region. b) The
measured applied load as a function of the displacement during the repeating loading and unloading at a constant displacement rate. c) The crack
growth behavior at the interface between the molybdenum oxide and silicon nitride layers in air at 30% RH and 70% RH and in water. d) XPS O1s peaks
of the molybdenum oxide surface in the pristine state and after the delamination of silicon nitride from molybdenum oxide.

the inset of Figure 3b. The DCB specimens were loaded and starts to grow, and E′ is the plane-strain modulus of the beam
unloaded with a constant loading speed of 0.2 µm s–1, and the (glass). B and h are the width and half-height, respectively, of the
applied force and the displacement were measured simultane- specimens. The adhesion energy between the silicon nitride and
ously. The critical load at which delamination starts to occur was molybdenum oxide layers was measured in lab air and determined
≈0.98 N as shown in Figure 3b, and it was confirmed that delam- to be 0.81 ± 0.08 J m–2 that was similar to the adhesion energy
ination occurred even with little force. The applied load (P) and between Cu and graphene (0.72 ± 0.07 J m–2). It is well known
displacement (δ) were utilized to calculate the crack length (a) that the layers of Cu and graphene can be easily delaminated.[26]
and the fracture energy (Gc) using the following equations: Since the adhesion between the barrier layer of the oxide TFTs
and the molybdenum oxide film was weak, the TFTs were easily
 CE ′Bh 3 
1/3 delaminated from the rigid substrate without leaving any residue.
a= − 0.64h (2) In addition, it is expected that the peel-off method can be imple-
 8 
mented in a large area, because the extracted adhesion energy of a
2 large size such as 6 G (1500 × 1850 mm) is small as 2.24 J.
12Pc2a 2  h The delamination of the oxide TFTs from the molybdenum
Gc = 2 3 
1 + 0.64  (3)
E ′B h  a oxide layer was ascribed to the environment-assisted subcrit-
ical debonding. This principle was validated by measuring
where C is the elastic compliance of specimen that can be the crack growth rates at the interface between the silicon
obtained from dδ/dP, Pc is the critical load at which the crack nitride and molybdenum oxide layers under various humidity

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conditions in air and in water. Figure 3c shows the variation where E i and hi are the effective Young’s modulus and the
in the measured crack growth rates with the applied debond thickness, respectively, of the ith layer. The effective Young’s
driving energy in air with a relative humidity (RH) of 30 and modulus was calculated using the following equation:
70% and in water at a fixed temperature, 30 °C. The relative
position of the curves was highly dependent on the RH and Ei
Ei = (5)
the environment. The curve corresponding to the debonding 1 − v i2
in water exhibited a low threshold debond driving energy (Gth)
of ≈0.30 J m–2. The Gth in air at an RH of 30% and 70% was where Ei and νi are the Young’s modulus and the Poisson’s ratio,
1.09 and 0.51 J m–2, respectively, showing clear decreasing respectively, of the ith layer. The elastic properties and the layer
trend of the Gth with increasing relative humidity. The sig- thicknesses for the system of the flexible oxide TFTs were as
nificant variation in the Gth with the relative humidity indi- follows: (1) Ecarrier = 20 GPa, vcarrier = 0.44, and hcarrier = variable,
cated that the interface between the silicon nitride and molyb- (2) EITO = 116 GPa, vITO = 0.35, and hITO = 0.15 µm, (3)
denum oxide layers was susceptible to interactions with the EAlOx = 370 GPa, vAlOx = 0.22, and hAlOx = 0.02 µm, (4)
water in air.[27] Therefore, the water content in the environ- EIGZO = 137 GPa, vIGZO = 0.36, and hIGZO = 0.02 µm, (5) same as
ment affected the debonding behavior between the silicon that of the third layer, and (6) ESiNx = 166 GPa, vSiNx = 0.23, and
nitride and molybdenum oxide layers. The high reactivity of hSiNx = 0.3 µm. The results of the calculation indicated that the
molybdenum oxide with H2O promoted the chemical reaction neutral plane moved in the device direction with the decrease
at the crack region. This facilitated the debonding and low- in the thickness of the carrier film.
ered the adhesive strength between the layers. Therefore, the The electrical characteristics of the oxide TFTs were
easy delamination of the TFTs was attributed to the reaction dependent on the property of the channel. Therefore, the
with H2O at the crack tip. applied strain at the interface between the active layer and the
The peaks in the XPS spectra of the delaminated surface gate insulator was determined based on the thickness of the car-
were analyzed to confirm the formation of the OH terminated rier film and the bending radius. The distance between the neu-
fracture surface owing to the environment-assisted debonding. tral plane and the channel region is indicated as x in Figure 4a.
Figure 3d shows the O1s peak for the molybdenum oxide sur- The applied strain was calculated by following equation:[31]
face before and after the delamination of the silicon nitride
layer. The XPS O1s spectra comprised peaks that corresponded x
ε= (6)
to the oxygen vacancies, the MO bonds, and the OC or OH R
bonds. The binding energies of the peaks corresponding to the
oxygen vacancy (≈531.8 eV) and OH (≈532.8 eV) were higher where ε is the applied strain at the channel region, and R is
than that of the peaks corresponding to the MO bond.[28,29] bending radius during delamination. The strain at the device
There was a significant increase in the binding energy shoulder region during the delamination was determined based on the
after the delamination of the silicon nitride layer from the thickness of the carrier film (Figure 4b). The graph indicated
molybdenum oxide layer. This was attributed to the generation that the decrease in the thickness of the carrier film causes
of OH at the molybdenum oxide surface after delamination. lower strain in the channel region of devices.
The deconvolution results of the O1s peaks and the calculated The changes in the transfer characteristics of the devices before
concentrations of the bonding states are presented in Figure S4 and after the delamination were investigated based on the thick-
and Table S1, Supporting Information, respectively. It was ness of the carrier film. Figure 4c,d presents the variation in the
inferred that structural defects such as dangling bonds were transfer characteristics of the TFTs for a thick and thin carrier film,
generated at the interlayer during the delamination of the sil- respectively, before and after delamination. The figures showed
icon nitride layer by the application of a physical force; in addi- that the transfer curve for the thick carrier film shifted to the nega-
tion, OH was also generated by the reaction with the H2O in tive direction after the delamination. In previous studies, when the
air. Therefore, the molybdenum oxide layer and the inorganic oxide TFTs are subjected to physical stress and strain, it has been
layer were easily delaminated owing to the generation of the demonstrated through technology computer-aided design (TCAD)
OH terminated fracture. analysis that the oxygen vacancies (Vo) are generated due to the
The characteristics of the oxide TFTs are affected signifi- break of bonding between metal and oxide, causing an increase
cantly by the mechanical force or deformation induced during of donor-like Vo+/Vo2+ states.[32,33] When the thick carrier film was
the delamination from a rigid substrate. Therefore, it is impor- utilized for the delamination of the oxide TFTs, numerous oxygen
tant to modify the thickness of the carrier film to place the neu- vacancies were generated owing to the high applied strain. This
tral plane close to the brittle device. A schematic of the mecha- resulted in the negative shift of the transfer curve. When the thin
nism of delamination and the position of the neutral plane is carrier film was utilized for the delamination of the oxide TFTs, a
presented in Figure 4a. A group of researchers led by Rogers low strain was induced in the channel region. This resulted in no
proposed that the position of the neutral plane is determined by significant changes in the transfer characteristics after the delami-
the following equation:[30] nation (Figure 4d). The separation between the neutral plane and
the device decreased with the decrease in the thickness of the car-
rier film. This resulted in the lowering of the applied strain at the
 i h
∑ E ihi  ∑ j =1h j − i 
N

 channel region. Therefore, the use of the thin carrier film induced
i =1
2
hneutral = (4) no significant changes in the electrical characteristics of the TFTs
∑
N
i =1
E i hi after delamination.

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Figure 4. a) Schematic illustration of the delamination of the oxide TFTs and the position of the neutral plane. b) The variation in the applied strain
at the channel region of the oxide TFTs with the carrier film thickness during the delamination, for various bending radii. The variation in the transfer
characteristics of the devices before the delamination and after the delamination and subsequent transfer to the PET substrate with the application of
c) thick and d) thin carrier films for delamination.

The optical and electrical characteristics of the flexible oxide distribution and the Gaussian fitting curves of the Von, field-effect
TFTs after the delamination and transfer are presented in mobility, and S.S. The oxide TFTs on the PET substrate exhibited
Figure 5. The optical transmittance of the PET substrate and an average Von of −1.02 V and a high mobility of 29.8 cm2 V–1 s–1.
that of the oxide TFT on the PET substrate were compared by The low S.S of 0.088 V dec–1 for the flexible and transparent oxide
ultraviolet-visible (UV–vis) spectroscopy to investigate the trans- TFTs indicated the existence of a few trap sites at the interface
parency of the transferred devices. The optical transparency between the active layer and the gate insulator.[37–39] The TFTs
of each sample was measured within a wavelength range of also exhibited highly saturated optimal output characteristics and
350–800 nm. The UV–vis transmittance spectra of the PET and no contact issues (Figure S6, Supporting Information).
the flexible devices are shown in Figure 5a. The transmittance When TFTs are operated as the backplane of displays, they
of the PET substrate was 88%.[34–36] The flexible oxide TFTs on must be stressed under a positive and negative gate bias.[40]
the PET substrate exhibited an average transmittance of greater Furthermore, the high transparency of oxide TFTs induces the
than 82% in the visible light region (400–700 nm). The inset of exposure to stress under light illumination.[41] The application
Figure 5a shows that the emblem behind the TFT was clearly vis- of a negative gate bias and illumination to the devices induced a
ible. This indicated the high transparency of the fabricated TFTs. negative Von shift. The flexible and transparent oxide TFTs were
The electrical parameters of the transparent and flexible subjected to a positive bias stress (PBS), negative bias stress
devices were determined from the transfer characteristics of the (NBS), positive bias illumination stress (PBIS), and negative
sixteen individual oxides TFTs on the PET substrate. Figure 5b bias illumination stress (NBIS). The resulting transfer curves
shows the 95% confidence interval for the mean values of the were obtained to determine the electrical stability of the TFTs.
turn-on voltage (Von), field-effect mobility, and subthreshold A positive and negative gate bias stress of 2 V (1 MV cm–1) and
swing (S.S). The flexible oxide TFTs were reasonably uni- −2 V (−1 MV cm–1), respectively, were applied. There were no
form after the delamination and the transfer to the PET sub- significant changes in the transfer characteristics by the appli-
strate. Figure S5, Supporting Information shows the histogram cation of the PBS (Figure 5c) and NBS (Figure 5d) for 10 000 s.

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Figure 5. a) The UV–vis transmittance spectra for the flexible device and the PET substrate. b) The mean of the Von, S.S, and field-effect mobility for
the 16 oxide TFTs on the PET substrate, with a 95% confidence interval. The variation in the transfer curves of the flexible oxide TFTs under the c) PBS,
d) NBS, e) PBIS, and f) NBIS for 10 000 s.

The fabrication and annealing of the TFTs without any tem- under a gate bias stress. When the TFTs were subjected to the
perature limitations facilitated the generation of high-quality PBIS, there were negligible changes in the transfer character-
interfaces and composite layers. Therefore, the TFTs exhibited istics. Meanwhile the exposure of TFTs to the NBIS resulted in
high electrical stability.[42,43] Figure 5e,f show the electrical sta- the transfer curve shift to the negative direction (1.09 V). The
bility of the oxide TFTs under the PBIS and NBIS, respectively. ionized Vo was generated from the deep states of the oxide
The samples were subjected to an illumination of 0.5 mW cm–2 semiconductors and trapped at the gate insulator to induce

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Figure 6. The transfer characteristics of the flexible and transparent oxide TFTs on the curved metal mold with various curvatures, where the bending
axis is a) perpendicular and b) parallel to the channel. The insets indicate the variation in the Von. c) The transfer curves and d) the variations in the
Von and S.S of the flexible device after the repetitive bending over several cycles with a bending radius of 3 mm.

the Von shift to the negative direction under the illumination TFTs were analyzed in the bending state with different bending
stress. Furthermore, the gate insulator, which contained a high radii and directions. Figure S7, Supporting Information shows
concentration of OH, induced a severe deterioration in the sta- the photographs of the system for the measurement of the elec-
bility of the devices under the NBIS. The diffusion of H, from trical characteristics of the flexible oxide TFTs in the bending
the OH in the gate insulator, into the active layer during the state with a bending radius of 1 mm. Figure 6a,b show the
thermal annealing of the devices resulted in the formation of a transfer curves of the bent oxide TFTs for various bending radii
non-bridging oxygen hole center (NBOHC) at the middle gap of with the bending axis perpendicular and parallel to, respec-
the gate insulator. The holes or the ionized Vo were trapped in tively, the channel direction. The flexible oxide TFTs exhibited
this NBOHC, thereby inducing the negative shift of the transfer typical transfer characteristics in the bending state without any
curve.[44,45] The use of aluminum oxide that was fabricated by significant changes in their electrical performance, regardless
thermal atomic layer deposition (ALD) as the gate insulator of the bending radius and direction. The variation in the Von of
in this study facilitated the realization of highly stable devices the flexible oxide TFTs with the bending radius is shown in the
under a positive gate bias stress. It has been demonstrated that insets of Figure 6a,b. When the bending axis was perpendicular
plasma-based techniques such as plasma-enhanced ALD for the and parallel to the channel direction, with a bending radius of
formation of gate insulators generate electron trap sites.[46,47] 1 mm, the Von shifted by only −0.04 and −0.01 V, respectively,
The shifting of the transfer curves under the NBIS was attrib- for the curved metal mold. Furthermore, the ultrathin nature of
uted to the high concentration of hydrogen in the aluminum the flexible substrate and the oxide TFTs facilitated the lowering
oxide that was fabricated by thermal ALD. The stability of the of the strain that was applied to the devices in the bending
devices under the NBIS, however, can be improved by opti- state, even at low bending radii.[18,48,49]
mizing the properties of the gate insulator. The mechanical durability of the oxide TFTs on the PET
The mechanical properties of the flexible and transparent substrate was determined by measuring the change in the
oxide TFTs were also investigated in this study. First, the transfer characteristics over several bending cycles. The sche-
transfer characteristics of the flexible and transparent oxide matic diagram of the bent flexible and transparent oxide TFTs

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in the inset of Figure 6c indicates that the device was bent in a (ITO) was deposited and patterned as a source/drain electrode. A
direction that was perpendicular to the channel direction with 20 nm-thick layer of Al-doped indium-tin-zinc oxide, which is a well-
a bending radius of 3 mm. Figure 6c,d show the variation in known oxide semiconductor with high mobility, was utilized as the
active layer. Prior to the formation of the gate insulator, oxygen plasma
the transfer characteristics of the devices and the measured treatment was conducted on the active layer under 200 W of power
electrical parameters, respectively, during the repeated bending for 9 min to modulate the carrier density. The formation of the gate
over 10 000 cycles. The Von and S.S exhibited minor changes insulator involved the deposition of a 20 nm-thick layer of aluminum
by 0.03 V and 0.001 V dec–1, respectively, during the repeated oxide by thermal ALD at 200 °C. ITO was deposited as the gate
bending over 10 000 cycles. Therefore, the flexible and trans- electrode. The fabricated TFTs were subjected to thermal annealing at
parent oxide TFTs that were fabricated by delamination and 300 °C under a vacuum to optimize their electrical characteristics by
curing the defects.
transfer exhibited a high mechanical durability at a bending
Delamination and Transfer of the Oxide TFT: The carrier film was
radius of 3 mm during the repeated bending over several cycles. formed by the spin casting of polyvinyl alcohol (PVA) on the fabricated
and annealed devices. The oxide TFTs were delaminated from the rigid
substrate with the application of a physical force (by hand) to the carrier
film; subsequently, the devices were placed on the carrier film. The oxide
3. Conclusions TFTs on the carrier film were transferred to a 5 µm-thick flexible and
transparent PET substrate with an adhesive layer. Subsequently, since
In this study, we demonstrated the fabrication of ultrathin flex-
the PVA carrier film was soluble in water, the carrier film was removed by
ible and transparent oxide TFTs by the technique of delami- rinsing with H2O to open the electrode pad and measure the electrical
nation and transfer. The high-performance oxide TFTs were performance.
fabricated on a rigid substrate without temperature limitations Fabrication of the DCB Specimen: The DCB specimens were fabricated
and transferred to a 5 µm-thick PET substrate. The devices by the deposition of a 100 nm-thick layer of molybdenum oxide on
exhibited optimal coverage on and attachment to various a glass substrate by reactive sputtering with a reactive gas mixture of
objects with complex surface profiles such as contact lens, argon and oxygen (Ar:O2 = 7:3). A 300 nm-thick layer of silicon nitride
was deposited on the molybdenum oxide layer by PE-CVD at 300 °C.
clothes, and human skin. The results of the DCB test con- Thereafter, the glass was attached to the silicon nitride layer using epoxy
firmed the low adhesion energy between the inorganic layer (353ND) by curing at 120 °C for 2 h. The width and length of the DCB
and the molybdenum oxide layer. The analysis of the crack specimens were 8 and 50 mm, and the thickness of the glass substrate
growth rates under various humidity conditions confirmed was 700 µm.
that the delamination was facilitated by the reaction with H2O
at the interlayer crack tip. The oxide TFTs on the PET substrate
exhibited a high optical transparency of greater than 81% and
Supporting Information
a satisfactory electrical performance with a high mobility of
37 cm2 V–1 s–1. The devices also exhibited a high electrical sta- Supporting Information is available from the Wiley Online Library or
bility under gate bias and illumination stresses. The ultrathin from the author.
flexible oxide TFTs possessed excellent mechanical properties;
furthermore, they showed a high mechanical durability over
10 000 cycles of repeated bending with a bending radius of Acknowledgements
3 mm. These thin film devices also showed reliable transfer
This work was supported by the Wearable Platform Materials Technology
characteristics in the bending state, regardless of the bending
Center (WMC) funded by a National Research Foundation of Korea (NRF)
radius and direction. This study demonstrated that flexible grant by the Korean Government (MSIT) (No. 2016R1A5A1009926).
oxide TFTs could be fabricated without temperature limitations This work was also supported by the National Research Foundation
by delamination and transfer using a suitable exfoliation layer. of Korea (NRF) grant funded by the Korea government (MSIT)
Furthermore, it is expected that the devices transferred to the (2018R1A2A3075518).
PET substrate could also be directly attached to various sub-
strates. This flexibility was attributed to the ultrathin nature
of the TFTs. The fabricated flexible oxide TFTs in this study Conflict of Interest
could be potentially applied to the development of next-gener-
ation deformable displays such as multi-foldable, rollable, and The authors declare no conflict of interest.
stretchable displays owing to their outstanding optical, elec-
trical, and mechanical properties.
Data Availability Statement
Research data are not shared.
4. Experimental Section
Fabrication of the Oxide TFT: The formation of the exfoliation layer
involved the deposition of a 100 nm-thick layer of molybdenum oxide Keywords
on a glass substrate by reactive sputtering with a molybdenum target.
Subsequently, a 300 nm-thick layer of silicon nitride and a 20 nm-thick attachable, delamination, thin films, transistors, ultrathin device
layer of aluminum oxide were deposited on the molybdenum oxide
layer by plasma-enhanced chemical vapor deposition and plasma- Received: April 12, 2021
enhanced ALD, respectively, at 300 °C. These layers acted as barriers Revised: May 24, 2021
and protected the oxide TFTs from contaminants. Indium-tin oxide Published online:

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