Lithium Tantalate Photonic Integrated Circuits For Volume Manufacturing

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Article

Lithium tantalate photonic integrated


circuits for volume manufacturing

https://doi.org/10.1038/s41586-024-07369-1 Chengli Wang1,2,3,4, Zihan Li2,3,4, Johann Riemensberger2,3, Grigory Lihachev2,3,


Mikhail Churaev2,3, Wil Kao2,3, Xinru Ji2,3, Junyin Zhang2,3, Terence Blesin2,3, Alisa Davydova2,3,
Received: 26 June 2023
Yang Chen1, Kai Huang1, Xi Wang1, Xin Ou1 ✉ & Tobias J. Kippenberg2,3 ✉
Accepted: 2 April 2024

Published online: 8 May 2024


Electro-optical photonic integrated circuits (PICs) based on lithium niobate (LiNbO3)
Open access have demonstrated the vast capabilities of materials with a high Pockels coefficient1,2.
Check for updates They enable linear and high-speed modulators operating at complementary metal–
oxide–semiconductor voltage levels3 to be used in applications including data-centre
communications4, high-performance computing and photonic accelerators for AI5.
However, industrial use of this technology is hindered by the high cost per wafer and
the limited wafer size. The high cost results from the lack of existing high-volume
applications in other domains of the sort that accelerated the adoption of silicon-on-
insulator (SOI) photonics, which was driven by vast investment in microelectronics.
Here we report low-loss PICs made of lithium tantalate (LiTaO3), a material that has
already been adopted commercially for 5G radiofrequency filters6 and therefore
enables scalable manufacturing at low cost, and it has equal, and in some cases
superior, properties to LiNbO3. We show that LiTaO3 can be etched to create low-loss
(5.6 dB m−1) PICs using a deep ultraviolet (DUV) stepper-based manufacturing
process7. We demonstrate a LiTaO3 Mach–Zehnder modulator (MZM) with a half-wave
voltage–length product of 1.9 V cm and an electro-optic bandwidth of up to 40 GHz.
In comparison with LiNbO3, LiTaO3 exhibits a much lower birefringence, enabling
high-density circuits and broadband operation over all telecommunication bands.
Moreover, the platform supports the generation of soliton microcombs. Our work
paves the way for the scalable manufacture of low-cost and large-volume
next-generation electro-optical PICs.

Next-generation ultrahigh-speed PICs based on electro-optical mate- increased application range of LiNbO3 PICs, the path to commerciali-
rials are poised to play a role in energy-efficient data centres, optical zation remains difficult. Unlike SOI technology, LNOI lacks a larger
communications, 5G and 6G radiofrequency filters and in particu- volume of consumer electronics driving its demand, resulting in eco-
lar in AI workload-driven high-performance computing, provided nomic limitations to its commercialization. By contrast, another fer-
that scalable low-cost manufacturing becomes possible. In the past roelectric material, LiTaO3, which has similar structural properties to
two decades, PICs based on silicon (silicon photonics) have rapidly LiNbO3, has entered the large-volume production stage, driven by its
transitioned from academic research to widespread use in telecom- applications in 5G filters13,14, and is projected to achieve a production
munications8 and data centres9. One crucial factor driving the com- capacity of 750,000 lithium tantalate-on-insulator (LTOI) wafers a year
mercial feasibility of this technological revolution is the high-volume by 2024 (ref. 15). This substantial volume enables considerable benefits
availability and cost-effectiveness of SOI wafers. These SOI wafers, in terms of low-cost production when adopting LTOI as a platform for
prepared using smart-cut (ion slicing) techniques10, enable the man- PICs, but PICs based on this material have not been reported to date.
ufacture of silicon photonics but crucially are more widely used in LiTaO3, as well as having a large production volume, exhibits compa-
consumer microelectronics. Globally, more than 3 million SOI wafers rable, or in some cases superior, properties to LiNbO3. LiTaO3 is an
are produced each year, with the wafer diameter being as large as oxygen octahedral ferroelectric crystal with a crystal structure that is
300 mm8. Using a similar technique, LiNbO3 has been fabricated into nearly identical to that of LiNbO3, replacing Nb atoms with the heavier
lithium niobate-on-insulator (LNOI) structures, offering an entirely Ta atoms. This change gives LiTaO3 not only a greater mass density
new class of ultrahigh-speed, low-voltage electro-optical PICs3,11,12 that but also stronger chemical bonds, resulting in increased strength and
can become key components in future energy-efficient communi- chemical stability16. The optical bandgap of LiTaO3 (3.93 eV) is larger
cation systems. Despite the tremendous scientific progress and the than that of LiNbO3 (3.78 eV)17–19, enabling nonlinear optical conversion

National Key Laboratory of Materials for Integrated Circuits, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, Shanghai, China. 2Institute of
1

Physics, Swiss Federal Institute of Technology Lausanne, EPFL, Lausanne, Switzerland. 3Center of Quantum Science and Engineering, EPFL, Lausanne, Switzerland. 4These authors contributed
equally: Chengli Wang, Zihan Li. ✉e-mail: [email protected]; [email protected]

784 | Nature | Vol 629 | 23 May 2024


a b c d Height
630
40

2.4 nm
Ion implantation 625
20

Thickness (nm)
620
Wafer bonding

y (mm)
0 615 e
x
610
LiTaO3
–20
Splitting 605
SiO2
–40 600
CMP –40 –20 0 20 40
x (mm)
f DLC deposition DLC etching IBE Redeposition cleaning
and mask stripping
CH4 → a–C + 2H2 C + 2O → CO2 Ar+
DLC
LiTaO3
SiO2
Si

g h i j

Fig. 1 | LTOI substrates and optical waveguides. a, Schematic of the LTOI deposition by plasma-enhanced chemical vapour deposition (PECVD) from the
wafer-bonding workflow showing hydrogen-ion implantation, bonding, methane precursor, DLC dry etching through oxygen plasma, and LiTaO3
splitting and chemical mechanical polishing (CMP). b, Photograph of the etching by argon ion-beam etching (IBE), followed by redeposition and mask
bonded wafer demonstrating uniform and defect-free bonding. c, Thickness removal. The layers are DLC (black), LiTaO3 (light blue), SiO2 (purple) and Si
map of the LiTaO3 thin film on the wafer. The x,y axes represent the distance (grey). Spheres show C (black), O (red) and Ar+ (green). g, Colourized scanning
from the wafer centre. d, Atomic force micrograph of the LiTaO3 thin film electron micrograph (SEM) of LTOI microring resonator (blue). Scale bar,
surface. Scale bar, 500 nm. e, High-resolution scanning transmission 50 μm. h, Colourized SEM of etched LTOI microring and bus waveguide
electron-microscopy image of the LiTaO3–SiO2 bonding interface. The arrow coupling section. Scale bar, 2 μm. i, Colourized SEM of etched LTOI waveguide
represents the x-cut crystal orientation. Scale bar, 2 nm. f, Schematic of the and sidewall. Scale bar, 2 μm. j, Colourized SEM cross-section of etched LTOI
fabrication workflow for LTOI optical waveguides, including DLC hard-mask waveguide (blue) on top of SiO2 bottom cladding (purple). Scale bar, 500 nm.

to the visible and even ultraviolet20-wavelength range. Furthermore, ‘whispering gallery’ mode resonators have been fabricated from LiTaO3
the material exhibits a greatly decreased optical anisotropy, that single crystals26, as a result of femtosecond laser direct writing27 or
is, the magnitude of the optical birefringence is reduced more than focused ion beam milling28, scalable manufactured PICs have remained
10-fold compared with LiNbO3, which suppresses mode mixing, as can an outstanding challenge.
occur in tight waveguide bends. Moreover, LiTaO3 features a similar Here, we overcome this challenge and implement what is to our
Pockels coefficient (r33 = 30.5 pm V−1) to the well-established LiNbO3 knowledge the first PIC platform using LTOI based on direct etching7,
(r33 = 30.9 pm V−1) with a moderately larger electrical permittivity, and demonstrate ultralow optical loss, electro-optical tuning, switching
ϵ33 = 43, implying that the modulation efficiency of the two materials through the Pockels effect and soliton-microcomb generation through
is expected to be almost identical. Furthermore, LiTaO3 benefits from the optical Kerr effect of LiTaO3. We achieve this by transferring the
a larger optical damage threshold, which is relevant for high-power diamond-like carbon (DLC)-based masking etching process, originally
applications. Of particular relevance for applications in the realm of developed for LiNbO3, to LiTaO3, and propose a new solution to remove
microwave-optical quantum transduction21,22, the nearly 10-fold-lower LiTaO3 redeposition, which highlights the flexibility of our process for
microwave loss tangent of LiTaO3 (refs. 23,24) is a promising avenue to the fabrication of a variety of ferroelectric photonics platforms. We
improve device performance to unity conversion efficiency, which has also demonstrate a DUV approach to electrode manufacturing. Taken
so far eluded efforts using LiNbO3 owing to the limited quality factors together, our work establishes a basis for scalable volume manufactur-
of microwave resonators22. Historically, despite the beneficial optical ing of ultrahigh-speed electro-optical PICs.
material properties, the use of LiTaO3 for optical modulators in optical
communication networks has been limited. One of the reasons is that
the Curie temperature of LiTaO3 (610–700 °C, depending on the Li:Ta LiTaO3 PICs
ratio) is much lower than the temperature needed for the fabrication The fabrication process for LTOI wafers and optical waveguides is
of optical waveguides by ion diffusion (typically more than 1,000 °C), depicted in Fig. 1 (details in Methods). The LTOI wafer was fabricated
which compounded the use of LiTaO3 for bulk modulators on the basis by the smart-cut technique14. The process flow is schematically illus-
of the ion diffused waveguide25. For this reason, legacy bulk modulator trated in Fig. 1a. In contrast to the well-established LNOI preparation
technology has used LiNbO3. However, the commercial use of LTOI in process, which uses helium-ion implantation with an energy greater
wireless applications, owing to its suitable acoustic properties, com- than 200 keV29, the fabrication of LTOI favours hydrogen ions with an
bined with the above optical properties, makes it an ideal platform implanted energy of 100 keV and a beam current ten times higher, as
for scalable manufactured electro-optical PICs, although such a use found in most commercial ion implanters, thereby simplifying the
has never been demonstrated or pursued. Although free-standing wafer production. The fabrication recipes of LTOI are more closely

Nature | Vol 629 | 23 May 2024 | 785


Article
a b c d 104
120

Normalized transmission
MHz

Response | F/FKerr (0)|2


48.8 Probe O = 1,545 nm
38.5
MHz 1.0 100
Hz Nabs/2S = 2.0 MHz
M Hz 102

Occurrence
M
39.3 50.8 80
MHz
41.2
M Hz M Hz 60
43.6 35.2 0.5 0
z
MH N0/2S 40
8.2
z 4
MH = 26.8 MHz 20
72.9 10–2
y

z 0 0
–500 0 500 0 20 40 60 80 100 103 104 105 106 107 108
Frequency (MHz) Frequency (MHz) Modulation frequency (Hz)

e f eo
g eo o eo
LiTaO3 TE00
z eo LiNbO3 TE00
T
2.05 LiTaO3 TM00

Effective index
LiNbO3 TM00
T
o o 2.00
y
TE00 TM00
1.95
0 30 60 90 120 150 180
Angle T (degrees)
h i
15 Dispersion fit 15 Dispersion fit

10 10
Dint/2S (GHz)

Dint/2S (GHz)
5 5

0 0
L C S E O L C S E O
–5 –5
180 190 200 210 220 230 240 180 190 200 210 220 230 240
Frequency (THz) Frequency (THz)

Fig. 2 | Optical characterization of LTOI PICs. a, Wafer-scale map of mean magnetic (TM00) mode profiles in LTOI. Scale bar, 1 μm. g, Numerical simulation
intrinsic loss, κ0/2π, for similar resonators. b, Normalized resonance of fundamental TE00 and TM00 optical-mode effective refractive indices of LNOI
transmission spectrum of an optical racetrack microresonator at 209.358 THz. (red) and LTOI (blue) as a function of the angle between the waveguide and the y
c, Statistical distribution of intrinsic loss, κ0/2π, of the optical racetrack axis of the x-cut LNOI or LTOI film. The reduced birefringence of LTOI precludes
microresonator. Mean = 40.4 MHz, median = 36.4 MHz. d, Nonlinear optical- unwanted birefringent mixing between fundamental TE00 or TM00 modes in
response measurement (solid red line) and fit (solid black line) of the thermo- thick waveguides. Arrows indicate birefringent mode mixing. h, Dispersion
optical (red dashed line) and Kerr (blue dashed line) nonlinear responses of profile of an LTOI racetrack microresonator with the waveguide cross-section
the optical microresonator, demonstrating ultralow optical absorption loss. 2 μm × 0.5 μm and a slab 100 nm thick. D1/2π = 82.234 GHz, D2/2π = 197.88 kHz.
e, Illustration of the LiNbO3 (red) strongly negative uniaxial and LiTaO3 (blue) L, C, S, E and O telecommunication bands are marked with vertical dashed lines.
weakly positive uniaxial crystal birefringence. For LiTaO3, ordinary refractive i, Dispersion profile of an LNOI racetrack microresonator with similar
index nLT.o = 2.119, extraordinary refractive index nLT.e = 2.123 and the difference cross-section and strong mode mixing at frequencies above 215 THz, which
ΔnLT = 0.004; for LiNbO3, ordinary refractive index nLN.o = 2.21, extraordinary occupies the E-band and the O-band in the optical communication.
refractive index nLN.e = 2.14 and the difference ΔnLN = −0.07. f, Illustration of the D1/2π = 80.83 GHz, D2/2π = 105.72 kHz.
curve angle, θ, and fundamental transverse electric (TE00) and transverse

aligned with the high-volume commercial production of SOI wafers, loss, α, of 7.3 dB m–1 for the unreduced LiTaO3 wafer that is used for
resulting in higher efficiency and lower costs in the production of LTOI optical applications. We also characterized the optical loss of the LTOI
than of LNOI. The fabricated LTOI wafer has a 4-inch (102 mm) size with platform fabricated from the reduced-LiTaO3 bulk wafers, known in
a surface roughness of 0.25 nm and a non-uniformity of less than 30 nm the filter industry as acoustic grade or black LiTaO3, which undergo
(Fig. 1b–d). The crystallinity of LiTaO3 and the LiTaO3–SiO2 interface an extra chemical reduction step, typically by annealing in carbon
remain of high quality after the completion of the production process, powder to minimize the pyroelectric effect31 (Methods and Extended
and so does the sharpness of the bonding interface, as can be seen Data Fig. 1). The LTOI fabricated from the reduced wafer exhibits an
in the high-resolution scanning transmission electron microscopy intrinsic loss rate κ0/2π = 42 MHz in the best field and a mean value
image (Fig. 1e). Photonic building blocks such as optical ring resonators of κ0/2π = 82 MHz across the whole wafer. This corresponds to losses
(Fig. 1g), racetrack resonators and waveguide spirals are also fabricated. α = 8.8 dB m−1 and α = 17.1 dB m−1, which is below the published losses
The lithography, dry etching and by-product cleaning processes were of the wafer-scale fabrication of LNOI PICs32, with an average loss of
optimized to achieve both favourable coupling regions (Fig. 1h) and 27 dB m−1, making our DUV-based process directly applicable to widely
well-defined, smooth sidewalls (Fig. 1i) of the LTOI PICs. As detailed in used mass-manufactured LTOI wafer substrates. An optical-resonance
Methods, the removal of non-volatile by-products for LTOI requires a transmission spectrum (D101_LT_A2_F1_C4_02_WG4) and fit is shown
different chemical than for LNOI7. The cleaved cross-section featur- in Fig. 2b, which indicates an intrinsic loss rate of κ0/2π = 26.8 MHz;
ing steep sidewall angles of almost 70° with respect to the surface is this corresponds to a propagation loss of α = 5.6 dB m−1 for unreduced
shown in Fig. 1j. LiTaO3. We also fabricated optical-waveguide spirals with a waveguide
Next, we characterized the LiTaO 3 PICs (D101_LT_A2) using cross-section of 1.75 μm × 0.6 μm and found a propagation loss of
frequency-comb calibrated tunable diode laser spectroscopy30 to deter- around 9 dB m−1 (Extended Data Fig. 2). A histogram of fitted intrinsic
mine the optical loss and absorption of optical microresonators with a loss rates for the microresonator is shown in Fig. 2c. The contributions
waveguide width of 2.0 μm across the 4-inch wafers (Fig. 2a). We find of optical absorption and scattering from bulk and sidewall imperfec-
mean intrinsic loss rates, κ0/2π, of between 35.2 MHz and 72.9 MHz with tions can be separated by thermal response spectroscopy33 (Fig. 2d). An
eight of the nine fields performing better than 50.8 MHz. The microres- intensity-modulated pump laser was tuned to the centre of the optical
onator intrinsic loss rate κ0/2π = 35.2 MHz corresponds to a propagation resonance, and the frequency-modulation response of the optical

786 | Nature | Vol 629 | 23 May 2024


a b c 10
20 MHz z PD

Resonance shift (GHz)


8 255 MHz V–1
OSC
PM
6 ECDL 1.2

Transmission
1.0
4 AFG 0.8
0.6
2 0.4
0 2 4 6 8
Frequency detuning (GHz)
0
0 10 20 30 40
DC offset (V)

d g 1.2
VS = 6.4 V
VS L = 1.6 V cm
1.0

Normalized transmission (Arb. units)


z
y
0.8

e f
0.6
Electro-optic S21 (dB)

0
0.4
VS = 7.6 V
–3 dB VS L = 1.9 V cm
–5 0.2

–6 dB 1,310 nm
0 1,550 nm
–10
0 10 20 30 40 50 0 5 10
Frequency (GHz) Voltage (V)

Fig. 3 | Electro-optical tuning and switching in LTOI. a, Colourized SEM of showing electro-optical tuning of an LTOI resonance. Each colour step
LTOI (blue) racetrack optical microresonator with gold electrodes (yellow). corresponds to an increase in DC tuning voltage of 5 V. d, Optical micrograph of
Scale bar, 300 μm. b, Colourized SEM of pulley resonator and bus waveguide 2.5 mm-long MZM. Scale bar, 200 μm. e, Colourized SEM of MZM waveguides
coupling section. Scale bar, 5 μm. c, Measured resonance shift as a result of and electrodes. Scale bar, 10 μm. f, Electro-optical bandwidth (S21 parameter,
tuning voltage. The linear fit indicates a voltage tuning response of 255 MHz V–1. measured as the power ratio) of MZM for a device length of 2.5 mm at a
Left inset: schematic of the measurement set-up for microresonator tuning wavelength of 1,550 nm. g, Normalized optical transmission as a function of
measurement with phase-modulation (PM) sideband calibration. ECDL, external applied voltage on travelling-wave electrodes at wavelengths of 1,310 nm and
cavity diode laser; AFG, arbitrary frequency generator; OSC, oscilloscope; PD, 1,550 nm, showing a voltage–length product,Vπ L, of 1.6 V cm at the O-band and
fast photodiode. Right inset: normalized cavity transmission measurement 1.9 V cm at the C-band.

microresonator resulting from the thermo-optical and Kerr effects was in excellent agreement with the results from our optical dispersion
read out with a second laser tuned to the side of another resonance. We measurement, Dint = ωμ − ω0 − (D1 × μ), where μ indicates the azimuthal
modelled the frequency dependence of the thermal effect arising from mode index for the mode with frequency ωμ, D1 is a free spectral range,
the optical absorption and the optical Kerr effect using finite-element Dint is an integrated dispersion and ω0/2π = 205 THz, for the LTOI (D101_
simulations and fitted the combined response33,34. We found that the LT_A2_F1_C4_WG4) and LNOI (D133_02_F2_C5_01_WG4) waveguides,
absorption limit of our LTOI microresonator is κabs/2π = 2.0 MHz, cor- which are depicted in Fig. 2h. The optical microresonators have similar
responding to an absorption-limited propagation loss of α = 0.4 dB m−1, anomalous dispersion, but the dispersion profile of the LTOI micro-
which is close to recent results obtained for LNOI34. Therefore, the resonator remains smooth over the full measurement span of 185 THz
main source of loss in our tightly confining LiTaO3 waveguides is scat- to 240 THz, whereas the LNOI microresonator exhibits striking mode
tering losses. mixing at frequencies above 215 THz. The birefringence complicates the
The optical birefringence of LiTaO3 is more than one order of mag- design of compact PICs and is useful only in some special cases, such as
nitude smaller than that of LiNbO3 (Fig. 2e) and therefore enables birefringence phase matching36. Adjustments to the waveguide geom-
the fabrication of thick waveguides without incurring mode mixing etry and working wavelength can weaken the mode mixing caused by
between the fundamental modes in waveguide bends7,35. Mode mixing strong birefringence in LNOI7,37, but such adjustments result in reduced
occurs in x-cut LiNbO3 waveguide bends when the TE mode transitions optical confinement and chip compactness. By contrast, LTOI offers
from the extraordinary (eo) to the ordinary (o) axes above a critical much lower birefringence, thereby providing greater flexibility in
LiNbO3 thickness that at a wavelength of 1.55 μm lies at around 700 nm waveguide design and manufacturing, and mode-mixing-free opera-
and at a wavelength of 1.3 μm lies at around 600 nm, largely indepen- tion over all telecommunications bands from 1,260 nm to 1,625 nm,
dently of the slab thickness or waveguide width. In contrast, the low ranging from the O to the L band. Furthermore, the resonance shift
and positive uniaxial birefringence of LiTaO3 precludes mode mixing induced by the photorefractive effect in an LTOI microresonator is
in x-cut waveguides with a horizontal-to-vertical aspect ratio greater nearly fivefold smaller than that in an LNOI microresonator (Extended
than one. We simulate the effective mode indices of the fundamental Data Fig. 3 and Methods), which is consistent with the results obtained
polarization modes of LNOI and LTOI for a waveguide thickness of from bulk crystals38.
600 nm, a waveguide width of 2 μm and a wavelength of 1.55 μm as
a function of the angle between the propagation and the eo crystal
axes (Fig. 2f,g). For LiNbO3, we found a crossing of the fundamental TE Electro-optical modulation
and TM modes at an angle of 25°, whereas no mode crossing is found To demonstrate the utility of the LTOI platform for electro-optics,
for an LTOI waveguide with the same dimension. This observation is we created a tunable high Q-factor microresonator. The resonator

Nature | Vol 629 | 23 May 2024 | 787


Article
a Wavelength (nm)
1,650 1,600 1,550 1,500
–30 Raman shift

Ipd (Arb. units)


1.0
Power (dBmW)

–40 0.5 Soliton step


–50
0
0 0.2 0.4 0.6 0.8 1.0
–60 Time (μs)

–70
180 185 190 195 200 205
Frequency (THz)

b c VCO
FPC d
–30 0° 1.0 y
CW pump z

Raman intensity
SSB
Power (dBmW)

–40 90° 270° EDFA 0.9

(Arb. units)
y
OSC z T = 0º
–50 PD 0.8 T = 90º
180° yz
FBG y
–60 ESA TE 0.7 Polarization
PD T
–70 0.6 z
OSA
180 185 190 195 200 205 0 20 40 60 80 100
Frequency (THz) Rotation angle (degrees)
e f

–30

RF power (dBmW)
–80
0
Power (dBmW)

90° 270°

Sff (dBc Hz–1)


–40
–120
–50 180° –50 –160
–60 –200 –100 0 100 200
Frequency at 30.1 GHz (kHz)
–70 –100

180 185 190 195 200 205 101 102 103 104 105 106
Frequency (THz) Frequency (Hz)

Fig. 4 | DKS generation in LTOI microresonators. a, Optical spectrum of a amplifier (EDFA). FBG, fibre Bragg grating; FPC, fibre polarization controller.
single soliton microcomb featuring a sech2-spectral profile with a 3 dB The soliton microcombs were analysed using an optical spectrum analyser (OSA)
bandwidth of 4.9 THz, corresponding to an FWHM pulse duration of 63 fs at a and the nonlinearly generated light and microwave beat notes were recorded
pulse repetition rate, frep, of 81 GHz. Inset, the light generated during the rapid with a PD and analysed with an OSC and electrical spectrum analyser (ESA),
laser scan measured by filtering out the pump light. The soliton step is marked respectively. d, Variation of the Raman intensity with different LTOI crystal
with light blue shading. Ipd, photodiode current. b, Optical spectrum of a single rotation angles. Inset, the angle between the orientation (z axis) and the
soliton with a repetition rate of 30.1 GHz; ΔTFWHM = 71 fs. Inset, the relative phase polarization of the excitation laser. e, Optical spectrum of a three-soliton state
position inside the microresonator. c, Optical setup for soliton generation in with a repetition rate of 30.1 GHz. Inset, three solitons inside the microresonator.
x-cut LTOI microresonators. The orientation and TE polarization are also ΔTFWHM = 52 fs. f, Single-side band-phase noise-power spectral density (Sff ) of a
indicated in the schematic diagram of the fabricated LTOI chip. Rapid laser scans 30.1 GHz microwave beat note generated from the multisoliton state in e. Inset,
were generated using a single-sideband modulator (SSB) and voltage-controlled spectrum of a microwave beat note with a resolution bandwidth of 30 Hz.
oscillator (VCO), continuous wave (CW) laser and an erbium-doped fibre

has a racetrack design with an apex radius of 100 μm and a straight for LNOI at 1,550 nm1,3, with similar electrode structures, as expected
section length of 400 μm (Fig. 3a) with a uniform waveguide width given that LiNbO3 and LiTaO3 have almost identical Pockels coefficients
of 2 μm and pulley-style coupling sections (Fig. 3b). Metal electrodes (Extended Data Table 1).
were fabricated using a DUV-lithography-based lift-off process that We then characterized the small-signal electro-optic bandwidth of
allowed us to manufacture electrodes with an alignment tolerance the fabricated devices (Methods). The measured 3 dB electro-optic
of less than 100 nm to the optical waveguide (Methods). We applied bandwidth was more than 40 GHz (Fig. 3(f)).
a voltage across two of the four electrodes to measure the voltage
tuning coefficient and measure the resonance position using an
external-cavity diode laser (ECDL) (Fig. 3c and Methods). We found Soliton-microcomb generation
a voltage tuning efficiency of 255 MHz V–1 using a single electrode pair, Finally, we investigated the LiTaO3 platform for soliton-microcomb
which corresponds to 510 MHz V–1 if both phase-shifter sections are generation. The strong optical confinement, high Q-factor, anomalous
modulated. We also fabricated a travelling-wave MZM composed of dispersion and substantial Kerr nonlinearity of our LTOI microresona-
two 50:50 adiabatic Y-splitters at either end and a push–pull optical tors make them naturally suitable for dissipative Kerr soliton (DKS)
waveguide phase-shifter pair with a length of 2.5 mm (Fig. 3d). The generation39,40. However, LiTaO3 is recognized as a Raman-active crystal-
waveguide width was 1.2 μm and the gap between the LiTaO3 waveguide line material, displaying multiple robust vibrational phonon branches
sidewalls and the gold electrode was 2.5 μm on each side (Fig. 3e). The in various polarization configurations41, which can have a detrimental
etching depth was 220 nm, leaving a 400 nm slab. This maintained a effect on soliton generation. This Raman interference presents a com-
consistent group refractive index, ng, of around 2.25 for both microwave mon challenge when attempting to generate solitons in ferroelectric
and optics waves. The transmission through the MZM with a 10 kHz crystal platforms. For instance, despite extensive research efforts,
triangular voltage sweep is plotted in Fig. 3g. The MZM can work at achieving solitons in the x-cut configuration of LNOI has remained
two communication bands of 1,310 nm and 1,550 nm simultaneously, elusive1,42. It is well known that the Raman effect is polarization depend-
owing to the use of the broadband adiabatic Y-splitter. The measured ent, typically exhibiting maximum strength when the pump light is
Vπ was 6.4 V for 1,310 nm and 7.6 V for 1,550 nm, corresponding to a polarized along the polar axis of the crystal1,17. We investigated such
VπL of 1.6 V cm and 1.9 V cm, respectively. The difference in VπL arises a polarization-dependent Raman effect in both x-cut LNOI and LTOI
mainly from the overlap difference between the optical modes and the (Methods). A reduction in Raman intensity was achieved when the
electric field at distinct wavelengths and increased optical frequency. polarization of incident light transitions from being parallel to the
The measured VπL of 1.9 V cm is similar to the state-of-the-art results y axis to being parallel to the z axis (the rotation angle θ changes from

788 | Nature | Vol 629 | 23 May 2024


0° to 90°; Fig. 4d). We therefore used racetrack microresonators with birefringence allows for the ultra-broadband dispersion engineering of
the straight waveguide section oriented along the z axis (θ = 90°) to LTOI waveguides and for electro-optical frequency comb generation,
minimize the Raman interference. This configuration ensures that the in which the bandwidth is limited by dispersion12 and birefringence48,
TE mode predominantly aligns with the non-polar y axis, as depicted and octave-spanning bandwidth has not yet been achieved. LTOI is
in the schematic chip diagram in Fig. 4c,d. We used the rapid single equally promising for the quantum transduction of single microwave
sideband tuning scheme described in ref. 43 to overcome thermal non- photons21,22, which has recently garnered attention as a way to overcome
linearities and initiate solitons at a pump power of 90 mW on-chip using the thermal bottlenecks of interfacing with superconducting quantum
ECDL and an erbium-doped fibre amplifier for pumping. The optical computers49, because the dielectric loss tangent of LiTaO3 (ref. 23) is
set-up for single-soliton generation is depicted in Fig. 4c (and described nearly 10-fold lower than that of LiNbO3 (ref. 24).
in Methods). We achieved single-soliton generation at pulse repeti-
tion rates of 81 GHz (D101_LT_A2_F9_C4_02_WG6, Fig. 4a) and 30.1 GHz
(D101_LT_A2_F3_C6_01_WG3, Fig. 4b). The full width at half-maximum Online content
(FWHM) spectral bandwidth of the 81 GHz single soliton is 4.9 THz, Any methods, additional references, Nature Portfolio reporting summa-
corresponding to a pulse duration of 63 fs. The 30.1 GHz single-soliton ries, source data, extended data, supplementary information, acknowl-
state features a bandwidth of 4.0 THz and supports a pulse duration of edgements, peer review information; details of author contributions
71 fs. Various multi-soliton states were also achieved, and we depict an and competing interests; and statements of data and code availability
example state with three solitons in Fig. 4e (D101_LT_A2_F2_C4_01_WG3). are available at https://doi.org/10.1038/s41586-024-07369-1.
In each of the ten tested devices with the orientation θ = 90°, solitons
were consistently generated. Conversely, none of the attempts to gen-
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39. Herr, T. et al. Temporal solitons in optical microresonators. Nat. Photon. 8, 145–152 credit to the original author(s) and the source, provide a link to the Creative Commons licence,
(2014). and indicate if changes were made. The images or other third party material in this article are
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optical microresonators. Science 361, eaan8083 (2018). to the material. If material is not included in the article’s Creative Commons licence and your
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790 | Nature | Vol 629 | 23 May 2024


Methods buffered hydrofluoric acid (step 2; Extended Data Fig. 5b) for a short
time. Metal deposition and the following photoresist lift-off created
LTOI wafer fabrication the metal electrodes (steps 3 and 4). As for the air cladding devices,
The thin-film LiTaO3 wafers were fabricated by ion cutting and wafer the SiO2 layer could be removed with another wet etching in buffered
bonding, starting with ion implantation into a 525-μm-thick bulk LiTaO3 hydrofluoric acid (step 5; Extended Data Fig. 5c).
wafer. Commercially available optical-grade and acoustic-grade bulk
LiTaO3 wafers were used. Both grades of wafer are congruent compo- Photorefractive effect comparison between LiTaO3 and LiNbO3
sitions and their cost is essentially the same. The difference between The measured LTOI (D101_LT_A2_F2_C3_02_WG2) and LNOI (D101_LN_
acoustic-grade and optical-grade LiTaO3 lies only in whether the mate- F2_C3_02_WG2) racetrack microresonators have identical waveguide
rial has undergone a chemical reduction process (typically annealed in dimensions of 2 μm × 0.5 μm and a slab thickness of 100 nm. Both
carbon powder)31: acoustic-grade LiTaO3 is reduced but optical-grade microresonators are uncladded and have the same free spectral range
LiTaO3 is not. Of the two, the optical-grade LiTaO3 wafers exhibited of 80 GHz. A CW pump laser was Pound–Drever–Hall locked to the
slightly better crystalline quality, evidenced by a narrower FWHM cavity resonance and the resonance shift over time was monitored by a
extracted from the X-ray radiation diffraction rocking curve (Extended wavemeter. During the experiment, the input optical power delivered
Data Fig. 1c,e). Hydrogen ions with an energy of 100 keV and a fluence by the input lensed fibre was maintained at 3 mW for both the LNOI
of 7.0 × 1016 cm–2 were implanted into a 4-inch x-cut bulk LiTaO3 wafer. and LTOI samples, which experienced identical fibre–chip coupling
An ion-damaged layer was introduced under the surface. Subsequently, losses of 6 dB per facet, resulting in an equivalent power of approxi-
the implanted wafer was flipped and bonded to a blank 525-μm-thick mately 0.75 mW in the bus waveguide for each sample. The extinction
high-resistivity silicon carrier wafer covered with 4.7-μm-thick thermal ratio and loaded linewidth of the resonances were determined using a
silicon dioxide. A subsequent thermal annealing step (190 °C for 10 h) frequency-comb-calibrated transmission curve measurement, as illus-
facilitated the separation of the residual bulk wafer and the exfoliated trated in Fig. 2b. Both the LNOI and LTOI samples exhibited an extinction
LiTaO3 thin film. After that, we performed edge removal of the LiTaO3 ratio of 50%. The loaded linewidth for the LNOI resonance was measured
thin film and chemical mechanical polishing to remove the rough and at 265.4 MHz (κ0/2π = 33.4 MHz and κex/2π = 232 MHz), whereas for
defect-rich layer of LiTaO3 that was strongly affected by H-ion implanta- the LTOI resonance, it was found to be 150.8 MHz (κ0/2π = 18.8 MHz
tion and thin the LiTaO3 film to the desired thickness of 600 nm. The and κex/2π = 132 MHz), indicating higher intra-cavity power for the
established process is adaptable to accommodate wafer sizes of 6 or LTOI sample. The resonance frequency shift, denoted as Δf, over
8 inches. time t, induced by photorefractivity, was modelled as a result of the
charge-accumulation process: Δf = Δf0(1 − e−t/T), where T represents
LTOI PICs fabrication the time constant of the charge accumulation process and Δf0 is the
We adapted and improved the DLC-based process recently dem- equilibrium photorefractive-induced frequency shift. The data pre-
onstrated for the LNOI platform 7 to fabricate LiTaO 3 PICs. The sented in Extended Data Fig. 3 show a notably smaller time constant,
process flow is schematically illustrated in Fig. 1f. First, we depos- T, and equilibrium shift, Δf0, for LTOI than for LNOI. This observation
ited a 30-nm-thick layer of Si3N4, a 480-nm-thick layer of DLC and a is consistent with results obtained from measurements in bulk LiTaO3
60-nm-thick layer of Si3N4 by PECVD as the main hard mask for sub- crystals, as previously reported38.
sequent IBE. Then we defined the photonic waveguides and compo-
nents by deep-ultraviolet stepper photolithography and transferred Electro-optical device characterization
the pattern first into a thin Si3N4 layer by fluorine-based dry etching Linear electro-optic tuning measurement was performed in the C-band
and subsequently into the DLC hard mask layer by oxygen-based and O-band using an ECDL. A fibre polarization controller was used to
dry etching in a reactive ion etcher. The main etch of the photonic ensure the excitation of the TE mode. The laser frequency was calibrated
device layer was performed by IBE removing 500 nm of LiTaO3 and with a 250 MHz phase modulation by detecting the sidebands around
leaving a 100-nm-thick continuous LiTaO3 slab across the wafer. After the resonance. A voltage was applied across two of the four electrodes
dry etching, it is known for LiNbO3 (ref. 7) that an extra wet etch- and an oscilloscope was used to record the shift of the resonance to
ing step with RCA-1 solution is needed because of the non-volatile achieve the measurement of the voltage tuning coefficient. For Vπ meas-
by-product accumulating on the waveguide sidewall. However, LiTaO3 urement, the MZM modulator was driven using a 10 kHz triangular volt-
exhibits not only a higher mass density but also stronger chemical age signal while real-time monitoring of the optical transmission signal
bonds (Extended Data Table 1), resulting in increased mechanical was done. The extinction ratio was measured to be 15 dB and could be
and chemical strength, so a method for removing by-products is further improved by using directional couplers. For the high-speed
not needed for LiTaO3. Here, we removed the LiTaO3 redeposition electro-optical bandwidth measurement, a pair of high-speed micro-
with a more-alkaline solution of 3:1 KOH(40%):H2O2(30%). After wave probes was used to deliver the microwave signal to the input
that, we annealed the wafer at 500 °C in an oxygen atmosphere port of the transmission line. The output of the transmission line was
and deposited a 2-μm-thick upper cladding with PECVD based on terminated with a load of 50 Ω. The light was coupled into and collected
a hydrogen-free precursor to avoid overtone absorption from optical out of the chip using tapered lensed fibres. The modulated optical
phonons of the Si–OH stretch vibration around 1.5 μm. The subsequent signal was pre-amplified and filtered through an erbium-doped fibre
chip release entailed processes involving dry etching of chip bounda- amplifier and a bandpass filter, then detected by a 50 GHz photodiode
ries in SiO2 using fluorine-based chemistry, additional etching of the (XPDV2120RA-VF-FP). The S21 response (ratio of powers) was measured
silicon carrier using the Bosch process, and backside wafer grinding. by a 67 GHz vector network analyser (VNA, R&S ZNA67).
Apart from the low-loss optical waveguides, high-quality electrodes
are also required for the PICs. We develop a DUV stepper-compatible Soliton and Raman measurement
lift-off process with a dielectric sacrificial layer (Extended Data Fig. 5a). We used a rapid single-sideband tuning scheme described previously43
After finishing the fabrication of the optical waveguides, we deposited to overcome thermal nonlinearities and initiate solitons at a pump
a SiO2 layer with PECVD (step 1) with a thickness that exceeds the power of 90 mW on-chip using an ECDL and an erbium-doped fibre
desired metal thickness for the lift-off process. Then the pattern amplifier for pumping. The optical set-up for soliton generation is
was defined by DUV-stepper lithography and transferred to the depicted in Fig. 4c. The microresonator had a waveguide cross-section
SiO2 by dry etching. It is critical to undercut the sacrificial layer for of 2 μm × 0.5 μm with a 100-nm-thick slab. Raman measurement
the lift-off process, which we performed by dipping the wafer into was performed using a confocal RM5 Raman microscope. A 532 nm
Article
excitation laser was pumped with a 20× air objective lens and the
Raman scattering signal was collected by the same objective. We used Code availability
a UHTS300 spectrometer with a grating of 1,800 grooves per mm. The code used to produce the plots in this paper is available at Zenodo
A half-waveplate was used to change the polarization direction of the at https://doi.org/10.5281/zenodo.10215427 (ref. 50).
excitation laser. The measured Raman spectra of x-cut LNOI and LTOI
for the excitation laser with polarization angles of 0°, 30°, 60° and 90° 50. Wang, C., & Kippenberg, T. J. Lithium tantalate photonic integrated circuits for volume
manufacturing. Zenodo https://doi.org/10.5281/zenodo.10215426 (2023).
with respect to the z axis are depicted in Extended Data Fig. 4a,b. Both
samples have several strong vibration phonon branches with large
Acknowledgements The samples were fabricated in the EPFL Center of
linewidths. Typical Raman peaks are labelled. The strongest peak at MicroNanoTechnology (CMi) and the Institute of Physics (IPHYS) clean-room. The LTOI wafers
517 cm−1 corresponds to the silicon substrate. The Raman intensity were fabricated in Shanghai Novel Si Integration Technology (NSIT) and the SIMIT-CAS.
becomes lower when the polarization of incident light transitions from This work has received funding from the National Natural Science Foundation of China
(62293521). T.J.K. acknowledges funding from the European Research Council grant 835329
being parallel to the z axis to being parallel to the y axis. Remarkably, (ExCOM-cCEO) and from the EU Horizon Europe research and innovation program through
this reduction is more pronounced in LTOI than in LNOI (Extended grant 101113260 (HDLN). J.R. acknowledges funding from the SNSF through Ambizione
Data Fig. 4c). We therefore used racetrack microresonators with the Fellowship 201923. C.W. acknowledges financial support from the China Scholarship Council
(202104910464). X.O. acknowledges the National Key R&D Program (2022YFA-1404601) from
straight waveguide section oriented along the z axis to minimize the the Ministry of Science and Technology of China.
Raman interference. This configuration ensured that the TE mode
predominantly aligned with the non-polar y axis, as depicted in the Author contributions C.W. and Y.C. fabricated the LTOI wafers with technical support from
K.H. and X.W. C.W. and Z.L. fabricated the devices. J.R., Z.L. and C.W. performed numerical
schematic chip diagram in Fig. 4c,d. simulations and designed the devices. C.W. and Z.L. characterized the samples. C.W., Z.L., G.L.,
J.Z., M.C., X.J., A.D., T.B. and W.K. performed experiments. J.R., C.W, G.L. and Z.L. analysed the
Material properties comparison between LiTaO3 and LiNbO3 data, prepared the figures and wrote the manuscript with input from all authors. T.J.K. and X.O.
supervised the project.
LTOI not only has the advantage of higher production volume but also
has similar or even better performance than LNOI, owing to the inher- Funding Open access funding provided by EPFL Lausanne.
ent properties of LiTaO3. A summary of a comparison of the material
Competing interests T.J.K. is a co-founder and shareholder of Luxtelligence SA, a foundry
properties of LiTaO3 and LiNbO3 is shown in Extended Data Table 1. All commercializing LiNbO3 PICs, as well as DEEPLIGHT SA, a start-up commercializing PIC-based
the properties listed correspond to the congruent compositions, which frequency-agile low-noise lasers.
are both more readily available and more widely used in various fields
Additional information
than their stoichiometric counterparts. Supplementary information The online version contains supplementary material available at
https://doi.org/10.1038/s41586-024-07369-1.
Correspondence and requests for materials should be addressed to Xin Ou or
Data availability Tobias J. Kippenberg.
Peer review information Nature thanks Detlef Kip and the other, anonymous, reviewer(s) for
The data used to produce the plots in this paper are available at Zenodo their contribution to the peer review of this work. Peer reviewer reports are available.
at https://doi.org/10.5281/zenodo.10215427 (ref. 50). Reprints and permissions information is available at http://www.nature.com/reprints.
a b c
Acoustic grade LT bulk wafers
Reduced (black)
NA 48 MHz 78 MHz
F7 F8 F9
Smart-cut
42 MHz 43 MHz 135 MHz
F6 F1 F2

63 MHz 123 MHz 130 MHz


F5 F4 F3

Rocking Angle (degree)

d e

39 MHz 39 MHz 49 MHz


F7 F8 F9

Smart-cut 43 MHz 42 MHz 51 MHz


F6 F1 F2
Optical grade LT bulk wafers
73 MHz 48 MHz 35 MHz
Unreduced (white) F5 F4 F3

17.4 17.42
Rocking Angle (degree)

Extended Data Fig. 1 | Optical loss of the acoustic and optical grade LTOI free spectral range. Figure shows the most probable values of the intrinsic loss
integrated photonic devices. (a) Photo of the bulk acoustic and optical grade rate κ0/2π for a resonator from every field. The test chip from one field on the
LiTaO3 wafers. The black and yellow wafers are reductive and original acoustic acoustic grade wafer was damaged before the measurement (shown as NA).
grade LiTaO3 bulk wafers, respectively. The white wafers are optical grade. (c) XRD rocking curve measured on the LiTaO3 (110) Bragg peak of the acoustic
(b) Wafer map of the optical loss of LiTaO3 microresonators fabricated on grade LTOI wafer after bonding and polishing. (d,e) Same as (b,c) but for optical
acoustic grade LTOI wafers. The resonators are 2 μm wide racetracks with 80 GHz grade LTOI wafer.
Article
a b

OFDR (20 dB/div.)


500 µm
3100 3200 3300 3400 3500 3600 3700 3800 3900
Distance x ng-1 (mm)
c d
13
OFDR (20 dB/div.)

12

Loss (dB/m)
11
10
9
8
7
3100 3200 3300 3400 3500 3600 3700 3800 3900 180 190 200 210 220 230 240
Distance x ng-1 (mm) Frequency (THz)
e f g 7520
OFDR (20 dB/div.)

7515
OFDR (20 dB/div.)

7510

(fs/mm)
7505 1
= 7516.3 fs /mm
1
= -163 fs 2 /mm

1
2
7500 3
= 602.93 fs /mm
3

7495
3020 3040 3060 3080 3100 3900 3920 3940 3960 3980 180 190 200 210 220 230 240
Distance x ng-1 (mm) Distance x ng-1 (mm) Frequency (THz)

Extended Data Fig. 2 | Linear loss and dispersion measurement. (a) Optical individual traces offset by 3 dB to highlight the linear fit for extraction of the
micrograph of LTOI spiral (D101_LT_A2_F2_C7_Spiral5) with a length of 39 cm optical propagation loss. (d) Optical propagation losses extracted from the
and a waveguide cross-section 1.75 μm × 0.6 μm. The rectangular footprint is fits in panel (c) showing a propagation loss of around 8 dB/m in the optical C-
5 × 2 mm2. (b) Segmented Fourier transform of the optical frequency domain and L-bands and around 10 dB/m in the O-band. (e,f) Same as panel (b) but
reflectometry (OFDR) signal showing the strength of the coherent optical highlighting the regions around the front and back facet reflections of the
backreflection as a function of the optical length. Colors encode the central chip. The colored markers point to the extracted position of the facet and are
wavelength of the segments and correspond to illustrations in panel (d). An used to infer the dispersion of the spiral. (f) Frequency-dependent optical
−1
optical distance of 88 cm can be identified according to the reflection peaks of group velocity vg = β 1 c = 2.25 of the waveguide spiral and fit of the anomalous
the front and back facets of the waveguide spiral chip. A minor fabrication dispersion profile of β2 = -163 fs mm−2. The dispersion contribution of the
defect is found at an optical distance of 3.36 m. (c) Same as panel (b) but 300 μm long tapers is neglected.
mW Power mW Power
a Meter Meter
Wave
PD PD
meter
FPC
PM Att. OSC
CW pump 99:1 90:10 75:25
Microresonator PD

PID
MIX
b
100

LiNbO3 measured
80 LiNbO3 experimental fit
LiTaO3 measured
Resonance Shift (MHz)

LiTaO3 experimental fit


60

40

20

0
0 10 20 30 40 50 60 70 80 90
Time (s)

Extended Data Fig. 3 | Photorefractive effect comparison between LiTaO3 the wavelength is monitored by a wavemeter. (b) Photorefractive-induced
and LiNbO3. (a) Schematic of resonance drifting measurement setup. A pump resonance frequency shift in LNOI (red) and LTOI (blue) microresonators.
laser is Pound-Drever-Hall (PDH) locked to the resonance microresonators and
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a c
1
LNOI 0°

E(8TO)
Intensity (Arb. units)

E(1TO)
30°
60°

A(4TO)
90°
0.9
LNOI

E(2TO)

Intensity Ratio
0.8
b
LTOI
A(1TO)


Intensity (Arb. units)

LTOI
30°

A(4TO)
60° z
90° 0.7 Polarization
E(1TO)

Orientation y
0.6
200 300 400 500 600 700 800 0 20 40 60 80
Raman shift (cm-1) θ (degree)

Extended Data Fig. 4 | Raman intensity comparison between LNOI and different polarization angles. The Raman intensity is obtained by integrating
LTOI. Raman spectra of (a) x-cut LNOI and (b) LTOI for the excitation laser with all peaks that correspond to LiNbO3 or LiTaO3 and is normalized. Inset
polarization angles 0°, 30°, 60°, 90° with respects to the z-axis. (c) Variation of illustrates the angles between the orientation and the polarization of the
the Raman intensity ratio of LNOI and LTOI for the excitation laser with excitation laser.
a
1. SiO deposition and 2. SiO dry and wet etching 3. Metal evaporation 4. Lift-off 5. SiO removal
photolithography
Metal
PR
SiO
LT
SiO
Si

b c

1µm
5 µm

Extended Data Fig. 5 | Scalable manufacturing process based on DUV is colored in red, silicon dioxide in pink, and silicon in blue. (c) SEM of fabricated
stepper lithography for thick high speed gold electrodes. (a) Fabrication electrodes and LiTaO3 waveguide. The gold is colored in yellow and LiTaO3 in
process flow of the electrodes. (b) Scanning electron micrography (SEM) of the light blue.
cross-section of a silicon dummy wafer after step 2 in panel (a). The photoresist
Article
Extended Data Table 1 | Comparison of the material properties of LiTaO3 and LiNbO3

The lattice constant, density, Curie point, bandgap, dielectric constant, refractive index, birefringence, electro-optic coefficient, optical damage threshold and coercive electrical field are
compared.

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