Vertical Full-Colour micro-LEDs Via 2D Materials-B
Vertical Full-Colour micro-LEDs Via 2D Materials-B
Vertical Full-Colour micro-LEDs Via 2D Materials-B
https://doi.org/10.1038/s41586-022-05612-1 Jiho Shin1,2,3,16, Hyunseok Kim1,2,16, Suresh Sundaram4,16, Junseok Jeong1,2,5,16, Bo-In Park1,2,
Celesta S. Chang1,2, Joonghoon Choi5, Taemin Kim6, Mayuran Saravanapavanantham2,7,
Received: 16 January 2022
Kuangye Lu1,2, Sungkyu Kim1,2,5, Jun Min Suh1,2, Ki Seok Kim1,2, Min-Kyu Song1,2, Yunpeng Liu1,2,
Accepted: 30 November 2022 Kuan Qiao1,2, Jae Hwan Kim1,2, Yeongin Kim1,2,8, Ji-Hoon Kang1,2, Jekyung Kim1,2, Doeon Lee9,
Jaeyong Lee1,2, Justin S. Kim10, Han Eol Lee1,2,11, Hanwool Yeon1,2,12, Hyun S. Kum1,2,6,
Published online: 1 February 2023
Sang-Hoon Bae1,2,10, Vladimir Bulovic2,7, Ki Jun Yu6, Kyusang Lee9 ✉, Kwanghun Chung3,13 ✉,
Check for updates Young Joon Hong5 ✉, Abdallah Ougazzaden4,14 ✉ & Jeehwan Kim1,2,15 ✉
Micro-LEDs (µLEDs) have been explored for augmented and virtual reality display
applications that require extremely high pixels per inch and luminance1,2. However,
conventional manufacturing processes based on the lateral assembly of red, green
and blue (RGB) µLEDs have limitations in enhancing pixel density3–6. Recent
demonstrations of vertical µLED displays have attempted to address this issue by
stacking freestanding RGB LED membranes and fabricating top-down7–14, but
minimization of the lateral dimensions of stacked µLEDs has been difficult. Here we
report full-colour, vertically stacked µLEDs that achieve, to our knowledge, the highest
array density (5,100 pixels per inch) and the smallest size (4 µm) reported to date.
This is enabled by a two-dimensional materials-based layer transfer technique15–18
that allows the growth of RGB LEDs of near-submicron thickness on two-dimensional
material-coated substrates via remote or van der Waals epitaxy, mechanical release
and stacking of LEDs, followed by top-down fabrication. The smallest-ever stack
height of around 9 µm is the key enabler for record high µLED array density. We also
demonstrate vertical integration of blue µLEDs with silicon membrane transistors for
active matrix operation. These results establish routes to creating full-colour µLED
displays for augmented and virtual reality, while also offering a generalizable platform
for broader classes of three-dimensional integrated devices.
Micro-light-emitting diodes (µLEDs) are considered ideal building integration of freestanding RGB LED membranes followed by top-down
blocks for augmented and virtual reality (AR/VR) displays owing to their fabrication7–14. However, conventional epitaxial lift-off techniques
small size and high level of brightness, which are crucial for near-eye for the production of freestanding LEDs can be inadequate for con-
and/or outdoor applications1,2. However, the realization of full-colour struction of the sub-10 µm pixels required for AR/VR displays21. Spe-
µLED displays via conventional mass transfer processes has been chal- cifically, conventional heteroepitaxy and laser lift-off processes for
lenging. These processes require the extraction of red, green and blue indium gallium nitride (InGaN)-based LEDs require a thick buffer under
(RGB) µLED chips from their respective epitaxial wafers—GaAs for the active layers to minimize lattice mismatch-induced dislocations22
red, and sapphire for green and blue LEDs, for example—followed by and prevent laser-induced damage23, respectively. As a result, these
consecutive precision transfers of R-, G- and B-LED chips for lateral LED films are 5–10 µm in thickness, which makes the fabrication of
assembly of RGB pixels19,20. Despite enormous improvement in resolu- sub-10 µm vertical µLEDs impractical because the high aspect ratio
tion, yield and throughput, these approaches have yet to yield µLED impedes high-resolution lithography. Slow rates of release processes
displays of sufficiently high pixel density. and limited reuse of costly wafers present additional concerns for man-
To address these issues, many researchers have developed µLED ufacturers. Consequently, there is a critical need for a lift-off technique
displays with vertically aligned RGB subpixels through monolithic that can yield freestanding LED membranes that are ultrathin, readily
1
Department of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA. 2Research Laboratory of Electronics, Massachusetts Institute of Technology,
Cambridge, MA, USA. 3Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA. 4CNRS, IRL 2958, GT−CNRS, Georgia Tech-Lorraine, Metz, France.
5
Department of Nanotechnology and Advanced Materials Engineering, Sejong University, Seoul, Republic of Korea. 6Department of Electrical and Electronic Engineering, Yonsei University,
Seoul, Republic of Korea. 7Department of Electrical Engineering and Computer Science, Massachusetts Institute of Technology, Cambridge, MA, USA. 8Department of Electrical Engineering
and Computer Science, University of Cincinnati, Cincinnati, OH, USA. 9Department of Electrical and Computer Engineering, University of Virginia, Charlottesville, VA, USA. 10Department of
Mechanical Engineering and Materials Science, Washington University in Saint Louis, St. Louis, MO, USA. 11Division of Advanced Materials Engineering, Jeonbuk National University, Jeonju,
Republic of Korea. 12School of Materials Science and Engineering, Gwangju Institute of Science and Technology, Gwangju, Republic of Korea. 13Institute for Medical Engineering and Science,
Massachusetts Institute of Technology, Cambridge, MA, USA. 14School of Electrical and Computer Engineering, Georgia Institute of Technology, Atlanta, GA, USA. 15Department of Materials
Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA. 16These authors contributed equally: Jiho Shin, Hyunseok Kim, Suresh Sundaram, Junseok Jeong.
✉e-mail: [email protected]; [email protected]; [email protected]; [email protected]; [email protected]
Green light
absorber PI sidewall
encap.
Red μLED
Ni/Au TCE
c
d
463 535 665
Intensity (AU)
G B R
10 μm
400 450 500 550 600 650 700
Wavelength (nm)
Fig. 1 | Vertically stacked, full-colour µLEDs enabled by 2DLT. a, Exploded of three vertical µLED pixels side by side. Insets, cross-sectional SEM images of
schematic illustration of a vertical µLED pixel, consisting of RGB µLEDs and the device across p-contact (top), mesa (middle) and n-contact layer regions
green and blue light-absorbing PI interlayers. Inset, exploded schematic (bottom). c, EL image of vertical µLED device in b emitting three different
illustration of a µLED consisting of µLED mesa structure, Ni/Au TCE, PI sidewall colours in the dark. d, Normalized EL spectra of RGB µLEDs with peak wavelength
encapsulation layer and Ti/Au metal electrodes. b, Optical microscope image of 665, 535 and 463 nm, respectively.
releasable and low-cost, to further advance vertical µLED microdisplay with silicon thin-film transistors (TFTs) for active matrix operation.
technology. Last, we show the utility of 2DLT in the construction of large-scale µLED
Here we demonstrate full-colour, vertically stacked µLEDs that displays via high-resolution, selective mass transfer of µLEDs fabricated
achieve the smallest size (4 µm) and highest array density (5,100 pixels on 2D materials.
per inch (PPI)) reported to date, to our knowledge. This is enabled by Figure 1a shows the overall architecture of vertically stacked µLEDs
two-dimensional materials-based layer transfer (2DLT) techniques15–18 (see Extended Data Fig. 1 for process flow). We performed remote epi-
that allow (1) epitaxy of ultrathin RGB LEDs (thickness: 1–2 µm) on 2D taxy of an AlGaAs-based red LED on a graphene-coated GaAs wafer,
material-coated substrates via either remote epitaxy or van der Waals and van der Waals epitaxy of InGaN-based green and blue LEDs on
epitaxy, (2) mechanical release of LED layers from 2D materials and hBN-coated sapphire substrates, which yielded single-crystalline
subsequent reuse of the substrate, (3) stacking via the use of adhe- RGB LED layers of thickness 1–2 µm. These were released from their
sive polymer layers and (4) top-down fabrication to yield vertical RGB substrates via the 2DLT process. The released LED membranes were
µLEDs. Our vertical µLEDs achieve a total thickness of around 9 µm, stacked using PI absorber-bonding layers in the ascending order of
which enables the fabrication of µLED arrays with record high density. bandgap energy, to minimize the absorption of light in the upward
Fast and precise mechanical release of LEDs from 2D materials allows direction (pointing towards the viewer). µLEDs fabricated on the
high-throughput production of µLEDs, and reusability of the wafer transferred membranes consist of transparent conductive electrodes
reduces material cost. We also developed wavelength-selective polyim- (TCEs), mesa structures, a sidewall encapsulation layer (about 300 nm)
ide (PI) absorbers (approximately 1.6 µm) that can serve as both adhe- and sputtered contact metals (Fig. 1a, inset; see Methods for detailed
sive interlayers and optical filters, preventing interference between procedures).
LED membranes and eliminating the need to incorporate additional To fabricate sub-10 μm vertical µLEDs, which are crucial for fully
optical elements. We show a small µLED display with a pixel pitch of immersive AR/VR microdisplays, total µLED height must be minimized
14 µm (roughly 1,800 PPI) consisting of blue µLEDs integrated vertically to reduce the aspect ratio and prevent errors during photolithography.
Intensity (AU)
n-Al0.65Ga0.35As: 350 nm 2 mA
Al0.36Ga0.64As 10–2
1 mA
n-GaAs: 700 nm 10–4
n-Al0.65Ga0.35As
n-GaAs 10–8
Gr –3 –2 –1 0 1 2 3 4 5 620 640 660 680 700
III–V substrate Voltage (V) Wavelength (nm)
200 nm 2 cm
Intensity (AU)
Stacked
0.6 mA
10–2 0.2 mA
n-GaN
n-GaN/n-AlGaN: 750 nm 10–4
10–6
n-AlGaN 10–8
hBN –3 –2 –1 0 1 2 3 4 5 480 520 560 600
Al2O3 Voltage (V) Wavelength (nm)
200 nm 2 cm
Intensity (AU)
Stacked
0.6 mA
10–2 0.2 mA
n-GaN
n-GaN/n-AlGaN: 750 nm 10–4
10–6
n-AlGaN 10–8
hBN –3 –2 –1 0 1 2 3 4 5 440 460 480 500 520
Al2O3 200 nm Voltage (V) Wavelength (nm)
2 cm
Current (mA)
150
0.6
100 0.4
y: 10 μm x: 10 μm 50 0.2
15 μm 0 0
0 –180 –90 0 90 180 –1 0 1 2 3 4 5
RMS roughness: 0.375 nm 1010
Φ (º) Voltage (V)
0001 2110
Fig. 2 | Ultrathin RGB LED membranes produced via 2DLT. a–c, Schematic Si wafers following vertical stacking (stacked, blue). m–o, Normalized EL
illustrations of the epitaxial structures of an AlGaAs-based red LED grown on spectra obtained from red (m), green (n) and blue (o) µLEDs fabricated on Si
graphene-coated GaAs wafer (a) and InGaN-based green (b) and blue (c) LEDs substrates under varying levels of injection current. p, AFM morphology image
grown on hBN-coated sapphire substrates. d–f, Cross-sectional STEM images of a used sapphire substrate after removal of residual hBN layer. q,r, EBSD map
of red (d), green (e) and blue (f) LEDs. g–i, Photographs of 2-inch-wafer-sized (q) and XRD Φ scan data (r) obtained from blue LED grown on reused sapphire
freestanding red (g), green (h) and blue (i) LED films on TRT. j–l, I–V curves of red substrate. s, I–V curves obtained from blue LED devices grown on pristine (red)
(j), green (k) and blue (l) µLEDs fabricated on respective epitaxial wafers (on-wafer, and reused (blue) sapphire substrates.
black), on Si wafers following layer transfer (non-stacked (non-stk), red) and on
However, it has proved extremely challenging to reduce the thickness addition of wavelength-selective dyes into the PI adhesion layer elim-
of vertical µLEDs due to inherent challenges in growing and handling inates the need to introduce optical filters to prevent interference
freestanding LED films of near-submicron thickness, and also in regard between LEDs. These modifications yield full-colour vertical µLEDs at
to bonding and prevention of cross-talk between LEDs. The use of 2DLT a height of around 9 µm and sub-10 μm size (see Fig. 1b for optical and
enables the preparation of ultrathin, single-crystalline LEDs due to cross-sectional scanning electron microscopy (SEM) micrographs and
the relaxation of epitaxial strain on slippery 2D surfaces22,24–28. The Supplementary Fig. 1 for energy-dispersive X-ray (EDX) elemental maps
With abs.
Intensity (AU)
60
B B Undesired
40 Blue abs. PL effect
Green abs. PI B Abs
20
B G
0
Non-stack No abs. With abs.
400 500 600 700 800 405 500 550 600
Wavelength (nm) Wavelength (nm)
b
EL, blue + blue abs. EL, green + green abs.
No abs. No abs.
With abs. With abs.
Intensity (AU)
Intensity (AU)
Blue abs. 460 500 Green abs. 520 600
Blue LED Green LED
440 460 480 500 520 480 520 560 600 640
Wavelength (nm) Wavelength (nm)
Fig. 3 | Prevention of PL via wavelength-specific, PI-based absorbers. illustrations (left) and recorded EL spectra (right) of a transferred, non-stacked
a, Optical transmission spectra of blue and green light absorber layers preventing blue µLED (non-stack, black), a blue µLED integrated on top of a green µLED via
colour modulation due to cross-talk between LED layers. b, Schematic a PI adhesive layer (no abs., red) and a blue µLED integrated on a green µLED via
illustrations and normalized EL spectra of blue (left) and green (right) µLEDs a blue absorber layer (with abs., blue). Error bars represent s.d. for at least three
coated with (with abs.) or without (no abs.) absorber layers, respectively. measurements.
Insets, magnified plots of EL spectra of absorber-coated µLEDs. c, Schematic
illustrating stack composition). Figure 1c shows an electroluminescence µLEDs (198 of 200 functional devices) illustrating the high yield of layer
(EL) microscopy image of three vertical µLEDs in parallel emitting dif- transfer and fabrication processes. Supplementary Fig. 4c shows the
ferent colours (see Supplementary Fig. 2 for details on the arrangement near-Lambertian radiation patterns of vertically stacked RGB µLEDs.
of metal contacts). EL spectra of RGB µLEDs (Fig. 1d) indicate peak Luminance of RGB µLEDs is in the range 104–106 cd m–2, which is suf-
wavelengths of 665, 535 and 463 nm, respectively. ficient for AR/VR display applications1 (see Extended Data Fig. 3 for
Schematic illustrations (Fig. 2a–c) and cross-sectional scanning measurements of luminance and efficiency and Supplementary Note 3
transmission electron microscopy (STEM; Fig. 2d–f) images illustrate for discussion). For blue and green µLEDs, the TCE helps spread current
the epitaxial structures of AlGaAs-based red LED on a graphene-coated on the less conductive p-GaN layer (Supplementary Fig. 5). Figure 2m–o
GaAs wafer and InGaN-based green/blue LEDs on hBN-coated sapphire shows the EL spectra of transferred RGB µLEDs under varying levels
wafers. The thickness of RGB LED films is 1.9, 1.1 and 1.0 µm, respectively. of injection current. The blueshift of peak wavelength for green LED
The LEDs retain single-crystallinity and smooth surface morphology, emissions with increasing current is due to the quantum-confined Stark
as shown by electron backscatter diffraction (EBSD), X-ray diffrac- effect, which is commonly observed for InGaN-based LEDs29.
tion (XRD) and atomic force microscopy (AFM) measurement results A highly intriguing feature of 2DLT is the reusability of costly
(Extended Data Fig. 2 and Supplementary Note 1). STEM images of the epitaxial wafers, which allows substantial reduction in µLED manu-
hBN–substrate interface and active regions for blue and green LEDs facturing cost. Unlike conventional lift-off techniques that require
confirm the formation of an ultrasmooth hBN layer and multiquantum chemical-mechanical polishing to recover an epi-ready surface30–32,
wells (MQWs), respectively, with EDX elemental maps confirming Al precisely defined crack propagation through 2D material in 2DLT
and In levels within the LED (Supplementary Fig. 3). LEDs grown on 2D ensures that the substrate remains undamaged through the exfolia-
materials can be peeled off readily using metal stressors and thermal tion process and can be recycled after removal of the residual 2D layer
release tapes (TRTs) due to their weak interaction with the substrate, (Supplementary Note 4). A simple dry transfer process completely
as illustrated in Supplementary Video 1 and photographs of exfoliated peels off the hBN layer from a used sapphire substrate, as indicated
2-inch-wafer-sized RGB LED membranes (Fig. 2g–i and Supplementary by the disappearance of B 1s and N 1s peaks in the X-ray photoelectron
Note 2). Mechanical robustness provided by the metal stressor allows spectroscopy (XPS) spectra shown in Extended Data Fig. 4a (Methods).
transfer and stacking of freestanding LED layers without damage. As AFM analysis shows RMS roughness of 0.375 nm for the substrate after
a result, the I–V characteristics and turn-on voltages of RGB µLEDs hBN removal (Fig. 2p). We subsequently grew hBN and blue LED on the
fabricated on their respective epitaxial wafers (Fig. 2j–l, black) are wafer and performed EBSD analysis (Fig. 2q), XRD Φ scan (Fig. 2r) and
comparable to those of µLEDs fabricated from transferred (red) and I–V curve measurement on fabricated µLEDs (Fig. 2s). EBSD and XRD
vertically stacked (blue) membranes. In Supplementary Fig. 4a,b, the data indicate that the blue LED grown on reused sapphire substrate is
photograph of exfoliated 2-inch-wafer-scale blue LED film with no sign entirely single-crystalline (0001) without in-plane rotations, and its I–V
of physical damage indicates the high yield of the exfoliation process, curve (blue) appears comparable to that of blue LED grown on pristine
with the optical microscope image and collective I–V curves of blue (red) sapphire substrate. SEM images of LEDs grown on pristine and
10 μm
R+G B+G R+B R+G+B
b c d Our RGB sRGB gamut
EL, purple, yellow, cyan EL, white DCI-P3 gamut
520
0.8 540
560
0.6
Intensity (AU)
Intensity (AU)
500 580
y
0.4 600
620
0.2
480
460
0
450 500 550 600 650 700 450 500 550 600 650 700 0 0.2 0.4 0.6 0.8
Wavelength (nm) Wavelength (nm) x
e
Pitch (μm) 20 × 30 17 × 18 10 × 15 8 × 12 7 × 10 5×7 5×5
PPI 1,000 1,500 2,000 2,500 3,000 4,100 5,100
OM images
10 μm
10 μm
EL images
10 μm
10 μm
Fig. 4 | 2DLT-enabled full-colour vertical ultrasmall µLEDs. a, EL microscopy space, plotted along with sRGB (dotted line and triangle) and DCI-P3 (dotted
images of vertical µLEDs illuminating red, green, blue, yellow, orange, cyan, line and square) colour gamuts. The position of the white EL in c is indicated by
pink, purple and white light via mixing of RGB colours. b, Representative a white circle at coordinates (0.314, 0.341). e, Optical and EL microscopy images
EL spectra of purple, yellow and cyan light emitted by vertical µLEDs. of vertical µLED arrays for near-eye display applications, with seven different
c, Representative EL spectrum of white light emitted by vertical µLEDs. sizes (PPI 1,000–5,100).
d, Chromaticity of vertical µLEDs (solid line and circle) in the CIE 1931 colour
reused wafers show comparable surface morphology (Extended Data respectively, as indicated by the optical transmission spectra shown
Fig. 4c,d). These results strongly support the reusability of sapphire in Fig. 3a. As coatings on LEDs they can completely quench respective
substrates following 2DLT. Epitaxial wafers used in remote epitaxy are target colour emissions while transmitting over 90% of non-target col-
also found to be reusable33. our emissions, as confirmed by schematic illustrations and EL spectra
An important consideration in the design of vertically stacked, in Fig. 3b and Supplementary Fig. 6, respectively. Most importantly,
full-colour µLEDs is the prevention of interference between LED lay- evidence of their effectiveness in preventing PL in the vertical stack
ers by absorption and re-emission, a phenomenon known as photolu- configuration is shown in Fig. 3c and Supplementary Fig. 7. Whereas
minescence (PL)8. Downward emissions from blue and green LEDs can green PL is observed in the EL spectra of a blue LED stacked on a green
induce PL in adjacent green and red LEDs, respectively, making them LED by a PI layer, it is absent in the EL spectra of a device containing
turn on simultaneously and introduce unwanted colour modulation. To a blue absorber layer. These PI-based absorber-bonding layers play
prevent this, we conceived PI-based blue and green optical absorbers a critical role in reducing the combined thickness of vertical µLEDs.
and inserted them as adhesive interlayers between G/B and R/G LEDs, The precise vertical overlap of RGB emission regions and the small
respectively, to block downward emissions (see Methods for detailed thickness of vertical µLEDs enable natural and high-resolution colour
procedures and Extended Data Fig. 5 for data on absorber optimiza- mixing. EL microscopy images (Fig. 4a and Supplementary Video 2)
tion). Blue and green absorbers are designed to strongly absorb blue illustrate homogeneous illumination of yellow, orange, cyan, pink,
(approximately 460 nm) and green light (approximately 540 nm), purple and white light by vertical µLEDs. Representative EL spectra of
Epitaxy of blue InGaN LED on hBN-coated sapphire substrate. Heterogeneous integration of full-colour vertical µLEDs
An Aixtron 3 × 2-inch wafer, close-coupled showerhead reactor Adhesive bonding of red AlGaAs LED on receiver substrate.
system grew the hBN layer and blue InGaN LED on an Al2O3 (0001) Plasma-enhanced chemical vapour deposition (PECVD) of SiO 2
substrate via metal-organic vapour-phase epitaxy (MOVPE). (500 nm; STS PECVD) on Si wafer (thickness: 380 µm; University
Triethyl-boron, trimethyl-gallium/triethyl-gallium, trimethyl-indium, Wafer), followed by photolithography, e-beam evaporation of Ti/Ni
trimethyl-aluminium and ammonia served as precursors for B, Ga, In, Al (15/150 nm) and lift-off, prepared the receiver substrate with align
and N, respectively, and silane and bis(cyclopentadienyl)magnesium keys. Both the receiver substrate and red LED on TRT were treated with
served as Si and Mg precursors for n- and p-doping of active layers, re- oxygen plasma (Anatech Barrel Plasma System), spin-coated with a
spectively. Epitaxy began with growth of the hBN layer (approximately 1 vol% aqueous solution of (3-aminopropyl)triethoxysilane (APTES,
3 nm) at 1,300 °C, followed by the n-AlGaN layer (approximately 250 nm; Sigma-Aldrich) at a speed of 3,000 rpm for 30 s and baked at 110 °C
Al mole fraction around 14 ± 2%) at 1,100 °C. The growth sequence for for 1 min. Receiver substrate was then spin-coated with PI precursor
active layers included an n-GaN bottom contact layer (500 nm), five (PI-2545, HD Microsystems) at 3,000 rpm for 30 s, partially cured at
periods of InGaN quantum well layer (2.5 nm; In mole fraction around 110 °C for 30 s, pressed against the LED film on TRT using a steel vice
15 ± 1%) and GaN barrier layer (12 nm), and a p-GaN top contact layer (Toolmaker’s vise, Tormach, Inc.) and partially cured on a hot plate at
(170 nm). Electron and hole carrier concentrations in Si- and Mg-doped 180 °C for 10 min. Thermal release of the TRT from substrate by heating
GaN layers were 5 × 1018 and 1 × 101 cm−3, respectively. at 150 °C, and full curing of the PI by pressing the sample in a vice and
placing it in a convection oven at 250 °C for 1 h, completed the bonding
Epitaxy of green InGaN LED on hBN-coated sapphire substrate. process. Wet etching in FeCl3 solution (MG Chemicals) and 5:1 buffered
The MOCVD system was used to grow InGaN/GaN MQWs and a p-GaN oxide etchant (BOE, J. T. Baker) removed Ti/Ni layers.
layer for green emission on top of an n-GaN/n-AlGaN/hBN/Al2O3 (0001)
substrate, prepared via the process described in the previous paragraph Fabrication of red AlGaAs µLEDs. Photolithography (AS200 i-line
for blue LEDs, using high-purity hydrogen (H2) or nitrogen (N2) as car- Stepper) and RIE using Cl2 gas first defined mesa structures and then
rier gas. Trimethyl-gallium, trimethyl-indium and ammonia served as the outer boundary lines of µLEDs. Spin-coating a PI precursor diluted
precursors for Ga, In and N, respectively, with bis(cyclopentadienyl) 1:1 by weight in 1-methyl-2-pyrrolidinone (NMP, Sigma-Aldrich) at a
magnesium as Mg precursor for doping of the p-GaN layer. Epitaxy speed of 3,000 rpm for 30 s, followed by curing at temperatures of 110,
began with the growth of MQWs consisting of two periods of the In- 150 and 250 °C for 1, 3 and 60 min, respectively, formed a thin coating
GaN quantum well (2.3 nm) and GaN barrier layers (21 nm) at 710 °C, of PI (about 300 nm). Photolithography and RIE using O2 gas partially
with growth rates of 0.22 Å s–1 for InGaN QW and 1.17 Å s–1 for the GaN exposed n- and p-type contact layers, and subsequent photolithogra-
barrier. NH3-rich ambient prevented thermal decomposition of the phy, DC sputtering of Ti/Au (15/150 nm; AJA Sputterer) and metal lift-off
n-GaN layer during temperature ramp-up. Growth temperature for completed n- and p-type metal interconnections.
the p-GaN top contact layer (200 nm) was 1,000 °C. Rapid thermal
annealing (RTA) at 800 °C for 5 min in N2 ambient activated the Mg Preparation of PI absorber layers. Dissolving visible yellow dye pow-
dopant in the p-GaN layer. der (Epolight 5843, Epolin) in PI precursor to form a 0.5 wt% solution
prepared the blue absorber precursor, and dissolving red visible ab-
Remote epitaxy of blue InGaN LED on GaN substrate. Both molecular sorbing dye (Epolight 5396, Epolin) in PI precursor to form a 1.0 wt%
beam epitaxy (MBE) and MOCVD were used to grow an InGaN-based solution prepared the green absorber precursor. Spin-coating pre-
blue LED via remote epitaxy. In an MBE chamber boron nitride (BN) was cursors on glass slides at a speed of 3,000 rpm for 30 s and curing at
grown on a GaN (0001) wafer at 760 °C, after which a 300-nm-thick GaN temperatures of 110, 150 and 250 °C for 1, 3 and 60 min, respectively,
buffer was grown at 820 °C in situ. Elemental boron and gallium, in ef- prepared PI absorber samples for ultraviolet-visible analysis (Extended
fusion cells, and nitrogen plasma served as precursors for B, Ga and N. Data Fig. 5).
The substrate was then transferred to an MOCVD chamber in which the
active layers for blue emission were grown in the order n-GaN bottom Integration of green and blue LEDs and fabrication of vertical
contact layer (400 nm), five periods of InGaN quantum well (2.3 nm) and µLEDs. Procedures almost identical to those described above for
GaN quantum barrier (21 nm), and p-GaN top contact layer (200 nm). layer transfer and fabrication of red µLEDs were used to integrate and
High-purity hydrogen (H2) or nitrogen (N2) was used as carrier gas. fabricate green and blue LED layers on top of red µLEDs; differences
spectral responsivity and the emission spectrum of each LED, yielded Author contributions Jeehwan Kim, A.O., Y.J.H., K.C. and K. Lee conceived the idea and
the luminance and external quantum efficiency (EQE) of each µLED directed the team. J.S. coordinated and designed the experiments and characterization. H.K.,
under forward bias40. Far-field radiation patterns for stacked μLEDs S.S., J.J., B.-I.P., J.C. and K. Lu developed and performed epitaxial growth of red, blue and green
LED films under the guidance of Jeehwan Kim, A.O. and Y.J.H. 2D material-coated substrates
were measured by driving each µLED at a constant current of 1 mA and were prepared by H.K., S.S., J.J., B.-I.P., K. Lu, Y.L., K.Q. and Jekyung Kim. T.K. developed Si TFTs
recording the photocurrent from a Si photodiode (Newport 818UV) under the guidance of K.J.Y. M.S. developed the set-up and codes for measurement of
Extended Data Fig. 2 | XRD, EBSD, and AFM measurements of ultrathin RGB LED films. g-i, EBSD analysis results for red (g), green (h), and blue (i) LED films.
LED films obtained via 2DLT. a-c, XRD 2θ-ω scan results for red (a), green (b), j-l, AFM morphology images for red (j), green (k), and blue (l) LED films.
and blue (c) LED films. d-f, XRD Φ scan results for red (d), green (e), and blue (f)
Extended Data Fig. 4 | Verification of reusability of sapphire substrates LED (LED exfol.; blue), and used sapphire wafer after removal of residual hBN
after 2DLT. a-b, XPS spectra of B 1s (a) and N 1s (b) regions for hBN-coated layer (hBN removal; red). c-d, SEM images of blue LEDs on hBN grown on
sapphire wafer (reference; black), used sapphire wafer following exfoliation of pristine (d) and reused (e) sapphire wafers.
Extended Data Fig. 6 | Si TFTs on silicon-on-insulator wafer. a, b, Optical characteristics of the silicon TFT with W/L of 1.5 μm/2.2 μm, driven at VDS of 2 V.
microscopy images of a 30 × 30 array of silicon TFTs fabricated on silicon-on- d, Output characteristics of a Si TFT showing current saturation at VGS values
insulator wafer. Each TFT has dimensions of 2.2 μm × 9.2 μm. c, Transfer ranging from 0.5 V to 2.5 V.
Extended Data Fig. 8 | Schematic illustrations and optical microscope which leaves behind the PR-coated chips on sapphire substrate that can
images of 2DLT-based, selective µLED mass transfer process for undergo cleaning and additional lift-off (step ii). The slippery surface of 2D
manufacturing large-scale displays. The process involves the fabrication materials, combined with photolithography-based selection approach,
of blue LED chips (size ~10 µm) on hBN-coated sapphire substrate (step i), enables facile yet highly resolved extraction of µLED chips among a
photolithography of a partially-developed photoresist (PR) pattern that densely-packed array (chip-to-chip separation ~10 µm). Cleaning the PR
exposes only the upper bodies of µLEDs to be transferred (step ii), deposition residue, transferring the µLEDs onto a secondary substrate, and removing Ni
of Ni stressor layer and attachment of handling tapes (step iii), and mechanical and underlying PI layers complete the process (steps v-vii).
lift-off of the exposed µLEDs via cleavage through the hBN layer (steps iv),
These include mono, dual, and full-colour µLED displays, as well as full-colour displays based on mono colour µLEDs coated with colour conversion (CC) layers.
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