Vertical Full-Colour micro-LEDs Via 2D Materials-B

Download as pdf or txt
Download as pdf or txt
You are on page 1of 21

Article

Vertical full-colour micro-LEDs via 2D


materials-based layer transfer

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]

Nature | Vol 614 | 2 February 2023 | 81


Content courtesy of Springer Nature, terms of use apply. Rights reserved
Article
a b
Blue μLED B
G
R
Blue light
absorber 10 μm 10 μm

Green μLED Ti/Au


electrodes
n

Green light
absorber PI sidewall
encap.

Red μLED
Ni/Au TCE

PI/Si substrate μLED mesa


structure

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.

82 | Nature | Vol 614 | 2 February 2023


Content courtesy of Springer Nature, terms of use apply. Rights reserved
a d g j m EL, red
p-GaAs: 250 nm p-GaAs I–V, red
102
p-Al0.65Ga0.35As: 350 nm On-wafer 5 mA

Current density (A cm–2)


p-Al0.65Ga0.35As 100 Non-stk 4 mA
Al0.36Ga0.64As: 300 nm
Stacked 3 mA

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

GaAs buffer 3.5 μm 10–6

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

b e h k I–V, green n EL, green


p-GaN: about 400 nm 102
p-GaN On-wafer 1.8 mA

Current density (A cm–2)


Non-stk 1.4 mA
2 × InGaN/GaN 100 1.0 mA
MQW

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

c f i l I–V, blue o EL, blue


p-GaN: 200 nm 102
p-GaN Current density (A cm–2) On-wafer 1.8 mA
100 Non-stk 1.4 mA
5 × InGaN/GaN
MQW 1.0 mA

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

p q r Φ Scan, blue (reused) s I–V, blue (reused)


AFM, used Al2O3 subs. (nm) Blue LED (reused)
3.3 1.0 Pristine
200
0.8 Reused
Intensity (count)

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

Nature | Vol 614 | 2 February 2023 | 83


Content courtesy of Springer Nature, terms of use apply. Rights reserved
Article
a EL, blue (stack)
c
100 EL measured Non-stack
B + G (PL) B No abs.
80
Transmission (%)

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

84 | Nature | Vol 614 | 2 February 2023


Content courtesy of Springer Nature, terms of use apply. Rights reserved
a Red Green Blue Yellow Orange Cyan Pink Purple White

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

Nature | Vol 614 | 2 February 2023 | 85


Content courtesy of Springer Nature, terms of use apply. Rights reserved
Article
purple, yellow, cyan and white emissions are shown in Fig. 4b,c. Fig- could expand the utility of vertical µLED technology to large-scale,
ure 4d shows the chromaticity of vertical µLEDs in the CIE 1932 colour flat-panel displays, establishing the overarching potential impact of
space, along with standard RGB (sRGB) and DCI-P3 colour gamuts. The 2DLT in the field.
colour space achieved by our µLEDs has 99.4 and 86.9% overlap with In summary, we have demonstrated the strategies for 2D
sRGB and DCI-P3, respectively, indicating the potential to cover the material-based epitaxy, layer transfer and heterogeneous integra-
full range of colours required for display applications. The CIE colour tion of ultrathin, single-crystalline RGB LED films in the construction
coordinates for RGB LEDs are (0.676, 0.285), (0.307, 0.656) and (0.145, of vertically stacked, full-colour µLED arrays with record high device
0.066), respectively, and RGB colour purities are 88.3, 90.5 and 94.1%, density. We have also demonstrated an active matrix display based on
respectively (see Supplementary Note 5 for calculation). A white circle blue µLEDs integrated vertically with Si TFTs, as well as a 2DLT-based
at (0.314, 0.341) denotes the position of the white EL shown in Fig. 4c. mass transfer process that could extend the utility of vertical µLEDs
The greatest strength of our vertical µLED technology is the potential to large-scale displays. The performance of vertical µLEDs could be
to substantially reduce the size and pitch of RGB µLEDs compared with further improved by the development of remote epitaxy-based blue
traditional displays featuring lateral subpixel layouts. To demonstrate and green LEDs with enhanced material and device characteristics
this, we fabricated arrays of vertical µLEDs with pitch (excluding back- (Extended Data Fig. 9 and Supplementary Note 6), transparent conduc-
plane) ranging from 20 × 30 µm2 (around 1,000 PPI) down to 5 × 5 µm2 tive oxides with higher transparency and distributed Bragg reflectors
(around 5,100 PPI), as shown in the microscopy images in Fig. 4e and combined with colourless adhesion layers that could eliminate the
Supplementary Fig. 8. To our knowledge, only Ostendo Technologies loss of downward LED emissions. The materials, device architectures
Inc. has reported sub-10 µm full-colour µLED displays13,14, with other and fabrication processes presented here have the potential to help
reports of 1,000+ PPI µLED displays being limited to either mono- realize full-colour, µLED-based AR/VR microdisplays, televisions and
chrome displays34–36 or full-colour displays based on colour conver- smartphone displays, as well as broad classes of three-dimensional
sion layers that compromise emission efficiency37,38. The µLED array integrated photonic, electronic and optoelectronic systems.
density achieved in this study is more than one order of magnitude
higher than the PPIs of self-emitting RGB µLED displays reported in the
literature (Extended Data Table 1) and in news articles (Supplementary Online content
Table 1). The range of µLED densities achieved by our technology will Any methods, additional references, Nature Portfolio reporting summa-
be sufficient to meet the exceptional demands of human vision for ries, source data, extended data, supplementary information, acknowl-
near-eye display2,21. edgements, peer review information; details of author contributions
A key element of functional displays is the capability to address indi- and competing interests; and statements of data and code availability
vidual LEDs via active matrix operation. To demonstrate this, we fabri- are available at https://doi.org/10.1038/s41586-022-05612-1.
cated 300-nm-thick silicon membrane TFTs on a silicon-on-insulator
wafer, which was integrated vertically with blue μLEDs obtained via 1. Lee, V. W., Twu, N. & Kymissis, I. Micro-LED technologies and applications. Inf. Disp. 32,
van der Waals epitaxy. Extended Data Fig. 6 shows a 30 × 30 array of 16–23 (2016).
Si TFTs with dimensions 2.2 μm × 9.2 μm × 300 nm, channel width/ 2. Zhan, T., Yin, K., Xiong, J., He, Z. & Wu, S.-T. Augmented reality and virtual reality displays:
perspectives and challenges. iScience 23, 101397 (2020).
length 1.5/2.2 μm, on-off ratio of 105 and current saturation at differ- 3. Gong, Z. Layer-scale and chip-scale transfer techniques for functional devices and
ent gate voltages. Layer transfer and fabrication of blue µLEDs on top systems: a review. Nanomaterials (Basel) 11, 842 (2021).
of Si TFTs, followed by electrical interconnection of each µLED with a 4. Wu, Y., Ma, J., Su, P., Zhang, L. & Xia, B. Full-color realization of micro-LED displays.
Nanomaterials (Basel) 10, 2482 (2020).
TFT, yielded an active matrix µLED display with pixel pitch of 14 µm 5. Marinov, V. R. 52-4: Laser-enabled extremely-high rate technology for µLED assembly.
(about 1,800 PPI; Extended Data Fig. 7a–c and Methods). Individual SID Symp. Dig. Tech. Pap. 49, 692–695 (2018).
µLEDs can be addressed by applying current to the p-contact of LED 6. Bower, C. A. et al. Emissive displays with transfer-printed assemblies of 8 µm x 15 µm
inorganic light-emitting diodes. Photon. Res. 5, A23–A29 (2017).
(VSS) while applying voltage to the gate to activate the TFT (scan line), 7. Chun, J. et al. Vertically stacked color tunable light-emitting diodes fabricated using
enabling display of the ‘mit’ logo (Extended Data Fig. 7d). To construct wafer bonding and transfer printing. ACS Appl. Mater. Interfaces 6, 19482–19487 (2014).
a full-colour µLED active matrix display, silicon membranes may be 8. Kang, C.-M. et al. Monolithic integration of AlGaInP-based red and InGaN-based green
LEDs via adhesive bonding for multicolor emission. Sci. Rep. 7, 10333 (2017).
similarly transferred39 and stacked to form vertical TFTs that can be 9. Kang, C.-M. et al. Hybrid full-color inorganic light-emitting diodes integrated on a single
integrated with vertical µLEDs, as outlined in Supplementary Fig. 9. wafer using selective area growth and adhesive bonding. ACS Photonics 5, 4413–4422
Such an integration scheme could maximize the pixel density of µLED (2018).
10. Jin, H. et al. Vertically stacked RGB LEDs with optimized distributed Bragg reflectors. Opt.
displays to potentially achieve the long-awaited fully immersive AR/ Lett. 45, 6671–6674 (2020).
VR displays. 11. Li, L. et al. Transfer-printed, tandem microscale light-emitting diodes for full-color displays.
Although AR/VR microdisplays are intriguing applications for µLEDs, Proc. Natl Acad. Sci. USA 118, e2023436118 (2021).
12. Mun, S.-H. et al. Highly efficient full-color inorganic LEDs on a single wafer by using
display manufacturers have greater financial motivations towards multiple adhesive bonding. Adv. Mater. Interfaces 8, 2100300 (2021).
µLED-based flat-panel displays for televisions, smartphones and other 13. El-Ghoroury, H. S., Chuang, C.-L. & Alpaslan, Z. Y. 26.1: Invited paper: quantum photonic
consumer electronics. Contrary to microdisplays, flat-panel displays imager (QPI): a novel display technology that enables more than 3D applications. SID
Symp. Dig. Tech. Pap. 46, 371–374 (2015).
require lower pixel density (100–500 PPI) and a larger display area (up 14. Yadavalli, K., Chuang, C.-L. & El-Ghoroury, H. Monolithic and heterogeneous integration
to 80 inches and beyond), making mass transfer the desired approach of RGB micro-LED arrays with pixel-level optics array and CMOS image processor to
(see Supplementary Fig. 10a for illustration of process flow)3,5. Cur- enable small form-factor display applications. In Proc. SPIE 11310, Optical Architectures
for Displays and Sensing in Augmented, Virtual, and Mixed Reality (AR, VR, MR) (eds Kress,
rently the major cost driver for these technologies is insufficient trans- B. C. & Peroz, C.) 113100Z (SPIE, 2020).
fer yield, in particular for smaller µLEDs3,4. We conceived a solution 15. Ayari, T. et al. Wafer-scale controlled exfoliation of metal organic vapor phase epitaxy
using 2DLT-based mass transfer of stacked µLED chips. Extended Data grown InGaN/GaN multi quantum well structures using low-tack two-dimensional layered
h-BN. Appl. Phys. Lett. 108, 171106 (2016).
Fig. 8 illustrates the selective transfer of blue LEDs (size: 10 µm) on a 16. Li, X. et al. Large-area two-dimensional layered hexagonal boron nitride grown on
hBN-coated sapphire substrate using partially developed photoresist sapphire by metalorganic vapor phase epitaxy. Crystal Growth Des. 16, 3409–3415 (2016).
17. Kim, Y. et al. Remote epitaxy through graphene enables two-dimensional material-based
patterns, Ni stressors and TRTs, which enables facile yet highly resolved
layer transfer. Nature 544, 340–343 (2017).
extraction of µLED chips among a densely packed array (chip-to-chip 18. Kim, H. et al. Impact of 2D–3D heterointerface on remote epitaxial interaction through
separation about 10 µm; Methods). Such a process can reduce the num- graphene. ACS Nano 15, 10587–10596 (2021).
19. Kim, H.-s et al. Unusual strategies for using indium gallium nitride grown on silicon (111)
ber of transfer events by a factor of three, thereby increasing both man-
for solid-state lighting. Proc. Natl Acad. Sci. USA 108, 10072–10077 (2011).
ufacturing yield and speed, as illustrated in Supplementary Fig. 10b. 20. Kim, T.-i et al. High-efficiency, microscale GaN light-emitting diodes and their thermal
Mass transfer of isolated vertical µLED chips (Supplementary Fig. 11) properties on unusual substrates. Small 8, 1643–1649 (2012).

86 | Nature | Vol 614 | 2 February 2023


Content courtesy of Springer Nature, terms of use apply. Rights reserved
21. LaValle, S. M. Virtual Reality (Cambridge Univ. Press, 2016). 34. Day, J. et al. III-nitride full-scale high-resolution microdisplays. Appl. Phys. Lett. 99, 031116
22. Kum, H. et al. Epitaxial growth and layer-transfer techniques for heterogeneous integration (2011).
of materials for electronic and photonic devices. Nat. Electron. 2, 439–450 (2019). 35. Meng, W. et al. Three-dimensional monolithic micro-LED display driven by atomically thin
23. Cheng, J.-H., Wu, Y. S., Peng, W. C. & Ouyang, H. Effects of laser sources on damage transistor matrix. Nat. Nanotechnol. 16, 1231–1236 (2021).
mechanisms and reverse-bias leakages of laser lift-off GaN-based LEDs. J. Electrochem. 36. Ludovic, D. et al. Processing and characterization of high resolution GaN/InGaN LED
Soc. 156, H640 (2009). arrays at 10 micron pitch for micro display applications. In Proc. SPIE 10104, Gallium
24. Jiang, J. et al. Carrier lifetime enhancement in halide perovskite via remote epitaxy. Nat. Nitride Materials and Devices XII (eds Chyi, J.-I. et al.) 1010422 (SPIE, 2017).
Commun. 10, 4145 (2019). 37. Chen, G.-S., Wei, B.-Y., Lee, C.-T. & Lee, H. Y. Monolithic red/green/blue micro-LEDs with
25. Journot, T. et al. Remote epitaxy using graphene enables growth of stress-free GaN. HBR and DBR structures. IEEE Photonics Technol. Lett. 30, 262–265 (2018).
Nanotechnology 30, 505603 (2019). 38. Park, J. et al. Electrically driven mid-submicrometre pixelation of InGaN
26. Bae, S.-H. et al. Graphene-assisted spontaneous relaxation towards dislocation-free micro-light-emitting diode displays for augmented-reality glasses. Nat. Photon. 15,
heteroepitaxy. Nat. Nanotechnol. 15, 272–276 (2020). 449–455 (2021).
27. Chang, H. et al. Graphene-driving strain engineering to enable strain-free epitaxy of AlN 39. Carlson, A., Bowen, A. M., Huang, Y., Nuzzo, R. G. & Rogers, J. A. Transfer printing
film for deep ultraviolet light-emitting diode. Light Sci. Appl. 11, 88 (2022). techniques for materials assembly and micro/nanodevice fabrication. Adv. Mater. 24,
28. Chen, Z. et al. Improved epitaxy of AlN film for deep-ultraviolet light-emitting diodes 5284–5318 (2012).
enabled by graphene. Adv. Mater. 31, 1807345 (2019).
29. Ryou, J. et al. Control of quantum-confined Stark effect in InGaN-based quantum wells.
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in
IEEE J. Sel. Top. Quantum Electron. 15, 1080–1091 (2009).
published maps and institutional affiliations.
30. Chen, J. & Packard, C. E. Controlled spalling-based mechanical substrate exfoliation for
III-V solar cells: a review. Sol. Energy Mater. Sol. Cells 225, 111018 (2021).
31. Zhang, B., Luo, C. & Li, Y.-F. Damage-free transfer of GaN-based light-emitting devices and Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this
reuse of sapphire substrate. ECS J. Solid State Sci. Technol. 9, 065019 (2020). article under a publishing agreement with the author(s) or other rightsholder(s); author
32. Bauhuis, G. J. et al. Wafer reuse for repeated growth of III–V solar cells. Prog. Photovolt. 18, self-archiving of the accepted manuscript version of this article is solely governed by the
155–159 (2010). terms of such publishing agreement and applicable law.
33. Kim, H. et al. Multiplication of freestanding semiconductor membranes from a single
wafer by advanced remote epitaxy. Preprint at https://arxiv.org/abs/2204.08002 (2022). © The Author(s), under exclusive licence to Springer Nature Limited 2023

Nature | Vol 614 | 2 February 2023 | 87


Content courtesy of Springer Nature, terms of use apply. Rights reserved
Article
Methods Trimethyl-gallium, trimethyl-indium and ammonia served as precur-
sors for Ga, In and N, respectively, and silane and bis(cyclopentadienyl)
2DLT of red, green and blue LEDs magnesium as Si and Mg precursors for n- and p-type doping of GaN,
Epitaxy of red AlGaAs LED on graphene-coated GaAs substrate. respectively. RTA at 800 °C for 5 min in N2 ambient activated Mg dopant
A metal-organic chemical vapour deposition (MOCVD) reactor with a in the p-GaN layer.
close-coupled showerhead design was used to grow red AlGaAs LEDs,
with nitrogen as carrier gas. Trimethyl-gallium, trimethyl-aluminium 2DLT. For red LEDs, electron-beam (e-beam) evaporation of Ti (30 nm)
and arsine served as precursors for Ga, Al and As, respectively, and followed by sputtering of a tensile-strained Ni stressor layer (4 µm)
dimethyl-zinc and disilane served as Zn and Si precursors for p- and via DC sputtering, attachment of a TRT (release temperature: 120 °C;
n-doping of active layers, respectively. The pressure level for all growths Revalpha, Semiconductor Equipment Corp.) and gradual release of the
was 100 Torr. The epitaxy process began with growth of a thin GaAs tape exfoliated the LED film at the LED–graphene interface. Reactive ion
nucleation layer on the graphene-coated substrate at 475 °C, followed etching (RIE; PlasmaPro 100 Cobra 300 System, Oxford Instruments)
by the full buffer at 650 °C at a growth rate of around 33 nm min–1. The using Cl2 gas etched away the GaAs buffer under the device layers. For
active layers were grown in the sequence n-GaAs bottom contact layer green and blue LEDs, e-beam evaporation of Ni/Au (10/10 nm) followed
(700 nm), n-Al0.65Ga0.35As lower barrier (350 nm), Al0.36Ga0.64As emit- by RTA in air at 450 °C for 3 min formed TCEs. Oxygen plasma treatment
ter layer (300 nm), p-Al0.65Ga0.35As upper barrier (350 nm) and p-GaAs for 1 min, DC sputtering of Al (3 µm), attachment of TRT and removal
top contact layer (250 nm), all at 700 °C and a growth rate of about of the tape exfoliated the LEDs. The choice of Al as a support layer was
33 nm min–1. Cooling down the reactor with arsine flow prevented sur- based on the high etch selectivity of Al etchant type D (Transene Com-
face desorption. pany Inc.) for Al over Ni/Au TCE.

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

Content courtesy of Springer Nature, terms of use apply. Rights reserved


included the use of green and blue absorber precursors rather than PI positioned 12 cm away from the surface of the µLED. The photodiode
precursor to transfer green and blue LED layers, respectively, and the was mounted on a manual goniometer, and the µLED was kept sta-
use of Al etchant type D to remove Al support layers. After transfer and tionary at the goniometer’s centre of rotation. The photodiode was
fabrication of all three LED layers, photolithography and RIE using O2 rotated around the stacked μLEDs, scanning from −90° to +90° at a
gas removed parts of the blue and green absorber layers to expose metal step size of 5°. A MultiLab 2000 XPS system (Thermo VG Scientific)
contact pads for green and red LEDs. Photolithography, DC sputter- using a Mg Kα source collected XPS spectra for hBN samples at room
ing of Ti/Au (15/400 nm) and lift-off electrically connected the three temperature. Peak energies were calibrated by the C 1 s peak at 284.8 eV.
n-contact metal pads for RGB LEDs. Photolithography, DC sputtering A Park Systems NX10 Atomic Force Microscope measured surface
of Ti/Au (15/100 nm) and metal lift-off formed a black matrix for the roughness using a non-contact mode. A UV/Vis/NIR spectrophotom-
samples shown in Fig. 4a. eter (Lambda 1050, PerkinElmer, Inc.) collected optical transmission
spectra for blue and green light-absorbing layers and also for Ni/Au
Reuse of sapphire wafer for van der Waals epitaxy of blue InGaN TCEs. A FEI Helios 660 Focused Ion Beam, with a final milling voltage
LED of 5 keV, prepared cross-sectional specimens of vertical µLEDs. Depo-
After exfoliation of the blue LED layer via 2DLT, e-beam evaporation sition of C and Pt layers before milling prevented ion beam damage.
and DC sputtering of Ni/Ni (20/1.5 µm), followed by attachment and Scanning electron microscopy–energy-dispersive X-ray spectros-
peeling off of TRT, exfoliated the remaining hBN layer on used sapphire copy elemental maps were taken using EDAX TEAM software. A Titan
substrate. Placing of the wafer in FeCl3 solution for 3 min removed Themis Z G3 Cs-corrected microscope equipped with Velox software for
residual Ni, preparing the wafer for additional growth processes. drift-corrected frame imaging and EDX analysis collected STEM images
and EDX elemental maps. The operating beam voltage was 200 kV in
Fabrication of Si TFT-integrated blue µLED array STEM mode. A ZEISS Merlin high-resolution SEM equipped with an
Chemical-mechanical polishing reduced the total thickness of the EBSD detector collected EBSD data at 20 kV and 10 nA and a working
silicon-on-insulator wafer (top Si 300 nm; buried SiO2 1 μm; Si handle distance of 15 mm. A Bruker D8 HRXRD equipped with a four-bounce
400 μm) before device fabrication. PECVD deposition of a silicon oxide Ge(022) incident beam monochromator, which eliminates all incident
layer (300 nm) followed by photolithography and RIE using CF4/O2 gas wavelengths except Cu Kα1 (λ = 1.540562 Å), collected XRD 2θ-ω and
defined the mask pattern for doping of source and drain contacts of Φ scan data.
the Si TFT. Solid-state diffusion of phosphorus at 900 °C, a drive-in
process at 950 °C and a cleaning process using BOE and piranha solu- 2DLT-based chip transfer
tion completed the doping. Photolithography and RIE using SF6 gas Photolithography and RIE using Cl2 gas defined the blue µLEDs and
defined the shape of each TFT. Atomic layer deposition of Al2O3 (roughly hBN layer, exposing the sapphire substrate underneath. Photolithog-
30 nm) on an oxygen plasma-treated sample formed the gate oxide, raphy via underexposure of ultraviolet light formed a photoresist
and subsequent photolithography and RIE using CF4/O2 gas exposed pattern that exposed the upper bodies of selected µLED chips but
the source and drain contacts. Photolithography, sputtering of Ti/Au not the sapphire substrate surrounding them. E-beam evaporation of
(15/130 nm) and metal lift-off formed the metal contact (for source) and Ti (40 nm) followed by DC sputtering of Ni (3.5 µm), followed by the
VDD lines. Spin-coating of a PI precursor diluted 1:1 by weight in NMP attachment of TRT, enabled the exfoliation of selected µLED chips
at 3,000 rpm for 30 s, followed by curing at temperatures of 110, 150 among the chip array. Dipping the sapphire substrate in remover PG
and 250 °C for 1, 3 and 60 min, respectively, formed a thin coating of PI (Kayaku Advanced Materials, Inc.) removed photoresist on the sub-
(roughly 300 nm). Photolithography and RIE using O2 gas exposed the strate, and RIE using O2 gas removed photoresist residue on the exfoli-
gate and drain contacts and subsequent photolithography, sputtering ated sample on TRT. Adhesive bonding procedures described above
of Ti/Au (15/130 nm) and metal lift-off formed the gate electrode and transferred selectively released µLEDs on TRT to a PECVD SiO2-coated
scan lines. The procedures described above for layer transfer and µLED Si wafer. Chemical wet etching in both FeCl3 and BOE removed Ti/Ni
fabrication were used to form an array of blue μLEDs on top of Si TFTs. layers, and photolithography and RIE using O2 gas etched away PI
Photolithography and RIE using O2 gas formed via holes exposing the surrounding µLEDs.
drain contacts of Si TFTs, and subsequent photolithography, sputtering
of Ti/Au (15/130 nm) and metal lift-off formed electrical interconnec-
tions between the n-GaN contact of blue LEDs with the drain contact Data availability
of Si TFTs, as well as with VSS lines. All data generated or analysed during this study are included in the
paper.
Device characterization
Spectroscopy equipped by the Renishaw Invia Reflex Micro Raman 40. Forrest, S. R., Bradley, D. D. C. & Thompson, M. E. Measuring the efficiency of organic
light-emitting devices. Adv. Mater. 15, 1043–1048 (2003).
system collected EL spectra for LEDs. A 50× objective lens collected
sample emissions, resolved using a 1,200 g mm–2 grating and a commer-
Acknowledgements The team at Massachusetts Institute of Technology (MIT) acknowledges
cial silicon CCD detector. Probe station (Signatone Corp.), equipped support from the National Science Foundation (award no. 2001231), the Defense Advanced
with a semiconductor parameter analyser (Agilent 4156C, Keysight Research Projects Agency Young Faculty Award (no. 029584-00001), the Air Force Research
Technologies) and camera system (connected to an optical micro- Laboratory (award no. FA9453-21-C-0717) and the US Department of Energy’s Office of Energy
Efficiency and Renewable Energy under the Solar Energy Technologies Office (award no.
scope for collection of images and videos), recorded the I–V curves DE-EE0008558). The team at MIT also acknowledges support, in part, by LG electronics and
of LEDs, transfer and output characteristics of Si TFTs, EL microscopy Rohm Semiconductor. The team at Georgia Tech-Lorraine acknowledges partial funding by
images and video recordings. A computer-controlled source meas- the French National Research Agency under the GANEXT Laboratory of Excellence project.
The work by Y.J.H., J.J. and J.C. was supported by a National Research Foundation of Korea
urement unit (Keithley 2636A) and a calibrated silicon photodiode grant funded by the Ministry of Science and ICT (nos. 2018K1A4A3A01064272, NRF-
(Thorlabs, no. FDS1010-CAL) recorded I–V characteristics and the pho- 2021R1A5A1032996 and 2022M3D1A2050793) and by the Ministry of Education (no.
todiode response of each µLED which, combined with photodiode 2022R1A6C101A774).

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

Content courtesy of Springer Nature, terms of use apply. Rights reserved


Article
luminance, EQE and radiation pattern under the guidance of V.B., and J.S., J.J., M.S. and J.H.K. Competing interests The authors declare no competing interests.
collected the data. J.S., H.K., J.J., M.-K.S., K. Lu, S.K., J.L., J.M.S., J.-H.K., J.S.K. and D.L. carried
out layer transfer and fabrication of LEDs. J.S. collected I–V curves, EL microscopy images and Additional information
optical transmission spectra. H.K., S.S. and K. Lu performed EBSD and XRD analyses. XPS and Supplementary information The online version contains supplementary material available at
AFM data were collected by K.S.K. EL spectra were obtained by J.S. and H.K. All SEM, EDX and https://doi.org/10.1038/s41586-022-05612-1.
STEM imaging and analyses were performed by C.S.C. J.M.S. designed all three-dimensional Correspondence and requests for materials should be addressed to Kyusang Lee, Kwanghun
schematic illustrations. H.E.L., H.Y., Y.K., H.S.K., S.-H.B. and K. Lee provided feedback Chung, Young Joon Hong, Abdallah Ougazzaden or Jeehwan Kim.
throughout experiments and data analysis. The manuscript was written by J.S., H.K., S.S., J.J., Peer review information Nature thanks Kazuhiro Ohkawa and the other, anonymous,
Y.J.H., A.O. and Jeehwan Kim. All authors contributed to the analysis and discussion of results reviewer(s) for their contribution to the peer review of this work.
leading to the manuscript. Reprints and permissions information is available at http://www.nature.com/reprints.

Content courtesy of Springer Nature, terms of use apply. Rights reserved


Extended Data Fig. 1 | Schematic illustrations of the 2D material-based layer transfer and vertical heterointegration process for constructing full-color
vertical µLEDs. The layers are transferred and stacked in the order of red, green, and blue LEDs using polyimide as adhesion layer.

Content courtesy of Springer Nature, terms of use apply. Rights reserved


Article

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)

Content courtesy of Springer Nature, terms of use apply. Rights reserved


Extended Data Fig. 3 | Luminance and external quantum efficiencies (EQEs) blue (g), and reference (h) µLEDs of varying size. Red, green, and blue µLEDs are
of RGB µLEDs. a-d, Measured luminance of red (a), green (b), blue (c), and obtained via 2DLT, while reference devices are blue µLEDs grown directly on
reference (d) µLEDs of varying size. e-h, Measured EQEs of red (e), green (f), sapphire substrate without 2D layer.

Content courtesy of Springer Nature, terms of use apply. Rights reserved


Article

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.

Content courtesy of Springer Nature, terms of use apply. Rights reserved


Extended Data Fig. 5 | Optimization of optical transmission characteristics thickness (represented as spin-coating rate) (d), and types of PI (colorless PI
of absorber interlayers. a-e, Optical transmission spectra obtained from from Kolon, Inc. and PI-2545 from HD Microsystems, Inc.) (e). Parameters in
absorber layers with varying concentrations of dyes dissolved in the PI parentheses represent conditions that apply for all data in each plot. (a, Insets)
precursor (a), film curing temperatures (b), types of dye product (c), film Photographs of representative absorber layers coated on glass slide.

Content courtesy of Springer Nature, terms of use apply. Rights reserved


Article

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.

Content courtesy of Springer Nature, terms of use apply. Rights reserved


Extended Data Fig. 7 | Si TFT-integrated blue InGaN μLEDs. a, b, Optical adhesive layer and electrically interconnected by sputtered metal. d, Optical
microscopy and tilted SEM images of a 30 × 30 array of blue μLEDs vertically images of the active matrix μLED display displaying the ‘mit’ logo. Scale bar,
integrated with silicon TFTs. c, Cross-sectional SEM image of a blue μLED 200 μm.
transferred on a 300 nm-thick silicon TFT on silicon-on-insulator wafer by PI

Content courtesy of Springer Nature, terms of use apply. Rights reserved


Article

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),

Content courtesy of Springer Nature, terms of use apply. Rights reserved


Extended Data Fig. 9 | Blue LED grown via remote epitaxy on GaN wafer. epitaxy. c, SEM images of the surfaces of GaN films grown via remote (left) and
a, Schematic illustrations of the epitaxial structures of InGaN-based blue LED van der Waals (right) epitaxy techniques. d-e, Measured EQEs and luminance of
grown on GaN wafer. b, AFM morphology image of a GaN film grown via remote blue µLEDs of varying size grown on GaN substrate.

Content courtesy of Springer Nature, terms of use apply. Rights reserved


Article
Extended Data Table 1 | Benchmark of vertically-stacked and laterally-assembled µLED displays

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.

Content courtesy of Springer Nature, terms of use apply. Rights reserved


Terms and Conditions
Springer Nature journal content, brought to you courtesy of Springer Nature Customer Service Center GmbH (“Springer Nature”).
Springer Nature supports a reasonable amount of sharing of research papers by authors, subscribers and authorised users (“Users”), for small-
scale personal, non-commercial use provided that all copyright, trade and service marks and other proprietary notices are maintained. By
accessing, sharing, receiving or otherwise using the Springer Nature journal content you agree to these terms of use (“Terms”). For these
purposes, Springer Nature considers academic use (by researchers and students) to be non-commercial.
These Terms are supplementary and will apply in addition to any applicable website terms and conditions, a relevant site licence or a personal
subscription. These Terms will prevail over any conflict or ambiguity with regards to the relevant terms, a site licence or a personal subscription
(to the extent of the conflict or ambiguity only). For Creative Commons-licensed articles, the terms of the Creative Commons license used will
apply.
We collect and use personal data to provide access to the Springer Nature journal content. We may also use these personal data internally within
ResearchGate and Springer Nature and as agreed share it, in an anonymised way, for purposes of tracking, analysis and reporting. We will not
otherwise disclose your personal data outside the ResearchGate or the Springer Nature group of companies unless we have your permission as
detailed in the Privacy Policy.
While Users may use the Springer Nature journal content for small scale, personal non-commercial use, it is important to note that Users may
not:

1. use such content for the purpose of providing other users with access on a regular or large scale basis or as a means to circumvent access
control;
2. use such content where to do so would be considered a criminal or statutory offence in any jurisdiction, or gives rise to civil liability, or is
otherwise unlawful;
3. falsely or misleadingly imply or suggest endorsement, approval , sponsorship, or association unless explicitly agreed to by Springer Nature in
writing;
4. use bots or other automated methods to access the content or redirect messages
5. override any security feature or exclusionary protocol; or
6. share the content in order to create substitute for Springer Nature products or services or a systematic database of Springer Nature journal
content.
In line with the restriction against commercial use, Springer Nature does not permit the creation of a product or service that creates revenue,
royalties, rent or income from our content or its inclusion as part of a paid for service or for other commercial gain. Springer Nature journal
content cannot be used for inter-library loans and librarians may not upload Springer Nature journal content on a large scale into their, or any
other, institutional repository.
These terms of use are reviewed regularly and may be amended at any time. Springer Nature is not obligated to publish any information or
content on this website and may remove it or features or functionality at our sole discretion, at any time with or without notice. Springer Nature
may revoke this licence to you at any time and remove access to any copies of the Springer Nature journal content which have been saved.
To the fullest extent permitted by law, Springer Nature makes no warranties, representations or guarantees to Users, either express or implied
with respect to the Springer nature journal content and all parties disclaim and waive any implied warranties or warranties imposed by law,
including merchantability or fitness for any particular purpose.
Please note that these rights do not automatically extend to content, data or other material published by Springer Nature that may be licensed
from third parties.
If you would like to use or distribute our Springer Nature journal content to a wider audience or on a regular basis or in any other manner not
expressly permitted by these Terms, please contact Springer Nature at

[email protected]

You might also like