Strongly enhanced second-order optical

nonlinearity in CMOS-compatible Al1−xScxN

thin films
Cite as: APL Mater. 9, 101104 (2021); https://doi.org/10.1063/5.0061787
Submitted: 29 June 2021 . Accepted: 09 September 2021 . Published Online: 04 October 2021

Valerie Yoshioka, Jian Lu, Zichen Tang, et al.

COLLECTIONS

Paper published as part of the special topic on Light and Matter Interactions

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APL Mater. 9, 101104 (2021); https://doi.org/10.1063/5.0061787 9, 101104

© 2021 Author(s).
 APL Materials ARTICLE scitation.org/journal/apm

Strongly enhanced second-order optical

nonlinearity in CMOS-compatible
Al1−x Scx N thin films
Cite as: APL Mater. 9, 101104 (2021); doi: 10.1063/5.0061787
Submitted: 29 June 2021 • Accepted: 9 September 2021 •
Published Online: 4 October 2021

Valerie Yoshioka,1 Jian Lu,1 Zichen Tang,2 Jicheng Jin,1 Roy H. Olsson III,2 and Bo Zhen1,a)

AFFILIATIONS
1
Department of Physics and Astronomy, University of Pennsylvania, Philadelphia, Pennsylvania 19104, USA
2
Electrical and Systems Engineering Department, University of Pennsylvania, Philadelphia, Pennsylvania 19104, USA

Note: This paper is part of the Special Topic on Light and Matter Interactions.
a)
Author to whom correspondence should be addressed: [email protected]

ABSTRACT
Silicon photonics has enabled large-scale production of integrated optical devices for a vast array of applications. However, extending its use to
nonlinear devices is difficult since silicon does not exhibit an intrinsic second-order nonlinearity. While heterogeneous integration of strongly
nonlinear materials is possible, it often requires additional procedures since these materials cannot be directly grown on silicon. On the other
hand, CMOS-compatible materials often suffer from weaker nonlinearities, compromising efficiency. A promising alternative to current
material platforms is scandium-doped aluminum nitride (Al1−x Scx N), which maintains the CMOS compatibility of aluminum nitride (AlN)
and has been used in electrical devices for its enhanced piezoelectricity. Here, we observe enhancement in optical second-order susceptibility
(χ (2) ) in CMOS-compatible Al1−x Scx N thin films with varying Sc concentrations. For Al0.64 Sc0.36 N, the χ (2) component d33 is enhanced to
62.3 ± 5.6 pm/V, which is 12 times stronger than intrinsic AlN and twice as strong as lithium niobate. Increasing the Sc concentration enhances
both χ (2) components, but loss increases with a higher Sc concentration as well, with Al0.64 Sc0.36 N exhibiting 17.2 dB/cm propagation loss at
1550 nm and Al0.80 Sc0.20 N exhibiting 8.2 dB/cm at 1550 nm. Since other material properties of this alloy are also affected by Sc, tuning the
Sc concentration can balance strong nonlinearity, loss, and other factors depending on the needs of specific applications. As such, Al1−x Scx N
could facilitate low cost development of nonlinear integrated photonic devices.
© 2021 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license
(http://creativecommons.org/licenses/by/4.0/). https://doi.org/10.1063/5.0061787

I. INTRODUCTION frequencies, frequency converters can enable communication

between systems that operate at different frequencies.9 Nonlinear
Integrated photonics is a growing field that manipulates light interactions can also be observed at a quantum level,10 allowing
signals using compact, chip-sized devices.1 Far-reaching applica- single-photon manipulation; in particular, spontaneous paramet-
tions range from telecommunication to sensing to optical comput- ric down conversion has been used to produce quantum photon
ing.2 While passive devices have proved useful in guiding light, pairs.11 Conversion between RF frequencies and optical frequen-
nonlinear devices are capable of controlling interactions between cies through the linear electro-optic effect can also be considered
different light signals in more complex processes,3 widening the a χ (2) nonlinear process; applications include quantum transduc-
capabilities of integrated photonic chips. tion9,12 and integrated electro-optic modulators.13 Optical signal
Second-order nonlinearities (χ (2) ) are used in frequency con- processing utilizes nonlinear processes such as difference frequency
version, modulation, and optical signal processing. Frequency generation for optical frequency mixing.14 Furthermore, cascaded
converters shift light sources to particular wavelengths;4–6 some χ (2) processes can act as stronger effective χ (3) processes for appli-
can tune the source to a desired wavelength within a limited cations that require higher order nonlinear processes, widening
range.7 Supercontinuum generators broaden spectral width using a their utility. While these processes can be performed with commer-
combination of nonlinear processes.8 By shifting signals to desired cial free-space optical components, nonlinear integrated photonic

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chips reduce device footprint and enable scalability for complex

systems.
Since the crystal structure determines χ (2) values, nonlinear
device performance is often limited by material choice. Additional
material limitations include bandgap, absorption loss, ease and cost
of fabrication, and compatibility with other materials. An impor-
tant subset of photonics uses silicon to successfully produce devices
on a large scale at low cost using techniques from CMOS facilities.
Other CMOS-compatible materials can be grown directly on sili- FIG. 1. Thin film characterization. (a) Cross-sectional SEM image of the
con or electrical chips, decreasing fabrication cost and complexity. Al0.64 Sc0.36 N film, with a thickness of 485.6 nm shown in green. (b) AFM image
Thus, CMOS compatibility is another important consideration that of the Al0.64 Sc0.36 N film; no anomalously oriented grains are present. See the
can impact ease and cost of fabrication, particularly on a large scale. supplementary material for SEM and AFM images of all samples.
Unfortunately, conflicting limitations can complicate material
choice. Silicon is clearly CMOS-compatible, but its centrosymmet-
ric structure precludes it from exhibiting χ (2) processes; its bandgap
of 1.1 eV also results in absorption of visible wavelengths.15 While spectroscopy (EDS) in a scanning electron microscope (SEM). High
accuracy for the SEM/EDS method is obtained by using a reference
many devices use lithium niobate (LN) due to its large χ (2) , with
d33 = 25 pm/V,16 it is not compatible with CMOS processes and
sample previously verified by Rutherford Backscattering Spectrom-
etry (RBS) for the k-factor analysis.26 The samples were grown on
cannot be directly grown on silicon platforms. Devices that utilize
100 mm diameter (100) Si wafers coated with 20 nm of (0001) Ti
lithium niobate with silicon often utilize wafer bonding, making
and 100 nm of (111) Pt. The bulk Al1−x Scx N was deposited with
large-scale production difficult.17 III–V materials, including GaAs
c-axis orientation perpendicular to the substrate, targeting a total
with one of the largest χ (2) values of d36 = 119 pm/V,16 can be
thickness of 500 nm; the thickness of each sample was confirmed
grown on silicon, but most face a multitude of challenges due
by cross-sectional SEM [Fig. 1(a)].
to lattice mismatch, different thermal expansion coefficients, and
We confirmed the quality of our samples, even at a high Sc con-
high growth temperatures.18 Several solutions include using buffer
centration, by AFM imaging Fig. 1(b) and measuring surface rough-
layers,19,20 growing silicon on III–V substrates,18 and wafer bond-
ness and full-width-half-maximum (FWHM) from x-ray diffraction
ing.21 However, these methods are not always CMOS-compatible
(XRD) rocking curves Table I. The AFM images confirm the lack
and require more complicated fabrication procedures. An excep-
of anomalously oriented grains,27 while low roughness over a large,
5 × 5 μm2 area and consistently sharp XRD curves indicate smooth,
tion to this difficulty is the III-nitride class, which could provide a
CMOS-compatible option due to their low-temperature sputtering
highly oriented films.25 These Al1−x Scx N films are nitrogen polar as-
process.22 However, these materials exhibit lower χ (2) , with AlN’s d33 deposited as they are readily etched using KOH,28 unlike metal polar
= 4 pm/V23 and GaN’s d33 = 10.3 pm/V.24 Furthermore, high-quality films. Furthermore, large piezoelectric electromechanical coupling
GaN samples often use a thin buffer layer of AlN grown on Si first to has been observed in these Al1−x Scx N materials,29,30 which would
reduce strain due to differing thermal coefficients.19,20 be diminished were there alternating domains oriented along the z-
Alloys provide a promising solution to tune and increase axis. As such, these films are strongly oriented and do not exhibit
χ (2) while maintaining CMOS compatibility. In particular, substi- competing domains of opposite polarity. The films are still poly-
tutional scandium (Sc) in Al1−x Scx N alloy thin films adjusts the crystalline since in-plane orientation of crystal domains is random
crystal structure and properties, notably increasing its piezoelec- despite strong orientation along the direction perpendicular to the
tric response.25 Al1−x Scx N’s development for electrical devices has substrate. While our samples were grown directly on Pt to enable
resulted in a robust, low-temperature fabrication process that pro- low-loss reflection SHG, the fabrication process can also be adapted
duces high-quality, wafer-scale samples. Unlike many other non- for dielectric substrates, including silicon and sapphire, for low-loss
linear materials, Al1−x Scx N is grown at low enough temperatures optical and optoelectronic applications.
to be CMOS-compatible and retains a relatively large bandgap.
However, its nonlinear optical properties in the visible and near-
infrared (NIR) regions have remained largely unexplored. Here, we III. THIN FILM REFLECTION SHG
report enhanced optical χ (2) of Al1−x Scx N thin films based on second To determine absolute χ (2) components, we utilize the relation-
harmonic generation (SHG) measurements. ship between the peak intensity of the fundamental light (I ω ) and
SHG (I 2ω ),31

II. FABRICATION 2ω2

I2ω = [ ][Tω2 T2ω T2ω ]deff
opt 2 2 2
Iω L , (1)
The Al1−x Scx N films were deposited in a pulsed DC physical ϵ0 c3 n2ω n2ω
vapor deposition system (Evatec CLUSTERLINE® 200 II) via co-
sputtering from separate 4-in. Al and Sc targets at 350C in a pure N2 where L is the total path length traveled in the sample, T ω (T 2ω ) is
environment with a gas flow of 20 SCCM. The power on the Al target the polarization-dependent power transmission coefficient of fun-
opt
was held at 1000 W while the power on the Sc target was adjusted to damental (SH) light through the air–sample interface, T2ω is the
reach the desired Sc concentration. Calibration of Sc cathode power effective power transmission coefficient of SH light through guiding
to Sc concentration was confirmed using energy dispersive x-ray optics after the sample, and deff is the effective nonlinear coefficient.

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TABLE I. Properties of Al1−x Scx N films studied in this work. Both rms roughness (Rq ) and average roughness (Ra ) were
measured over a 5 × 5 μm2 area and are low for all samples, indicating smooth films for optical measurements. Films are
relatively thin, ranging around 440–490 nm. The low full-width-half-max (FWHM) of x-ray diffraction (XRD) curves indicates
highly oriented films. Refractive indices at 1550 nm (nω ) and 775 nm (n2ω ) slightly increase with the Sc concentration.

Sc (%) Rq (nm) Ra (nm) t (nm) XRD FWHM (deg) nω n2ω

0 2.68 2.16 480 1.405 2.05 2.07
10 2.33 1.89 479 1.735 2.06 2.08
20 1.97 1.59 474 1.619 2.14 2.16
28 2.05 1.64 445 1.624 2.15 2.18
36 1.80 1.44 486 1.695 2.21 2.24

Power transmission coefficients were calculated using Fresnel equa- 0.01 mm2 based on knife edge measurements. The polarization was
tions; complete reflection from the Pt substrate for both wavelengths controlled to be either p- or s-polarized using two crossed polariz-
was assumed. ers. The reflected light signal at 775 nm was directed to a calibrated
The effective nonlinear coefficient deff is determined by crystal power sensor for absolute power characterization or a spectrometer
symmetry. Al1−x Scx N exhibits a wurtzite structure (6 mm group),25
so its nonzero χ (2) components are d33 , d31 = d32 = d15 = d24 using
condensed notation and Kleinman symmetry.32 In reflection geom-
etry, shown in Fig. 2(a), input polarization (p or s) determines how
each component contributes to deff ,

deff, p = d33 × sin2 θω sin θ2ω × f p (G1 )

+ d31 × cos2 θω sin θ2ω × [2 f p (G3 ) + f p (G2 )], (2)

deff, s = d31 × sin θ2ω × f s (G1 ), (3)

where θω (θ2ω ) is the angle of refraction for fundamental (SH)

light and f terms are polarization-dependent correction factors that
account for interference and multiple reflections, as defined in Sec. I
of the supplementary material. In the absence of interference, these
correction factors each equal one, recovering the typical equation for
effective χ (2) components in wurtzite films (Ref. 23). Although the
samples are polycrystalline in the crystal plane, the in-plane polariza-
tion components of p- and s-polarized fundamental light contribute
to the SH signal, which is p-polarized in both cases.
L is calculated using cross-sectional SEM thickness measure-
ments in Table I and angle of refraction. The effective refractive
index was determined via ellipsometry and prism coupling (Table I);
additional details are provided in Sec. II of the supplementary mate-
rial. Samples with a higher Sc concentration have a slightly higher
refractive index, which is consistent with other measurements of
the refractive index.33 Dispersion is minimal as the difference in
the refractive index at the fundamental and SH wavelengths is
∼0.02–0.03. Birefringence likewise has a negligible effect; additional
details are provided in Sec. III of the supplementary material. By
comparing the relative strength of the SH signals induced by p-
FIG. 2. Schematic of the SHG measurement technique. (a) SHG reflection geom-
and s-polarized fundamental light, we extract d33 and d31 using
etry in the crystal frame of reference. The sample thickness is t, refracted angle of
Eqs. (1)–(3). SH light is θ2ω , and polarization is labeled p and s. The SHG is p-polarized regard-
We measured the polarization-dependent reflected SHG from less of input polarization due to crystal symmetry. Multiple reflections are shown
each sample using the setup shown in Fig. 2(b). Source light from as their interference has a non-negligible effect. (b) SHG measurement appara-
an optical parametric amplifier pumped by a Yb:KGW laser ampli- tus. ND: neutral density filter, P: polarizer, L: lens, S: Al1−x Scx N sample, FM: flip
fier (PHAROS, Light Conversion) at 1550 nm with a 159 fs pulse mirror, F: filter, and PM: power meter. The SH signal is separated from fundamen-
tal light using a high-pass filter or a prism for spectra and power measurements,
duration and 3 kHz repetition rate was incident upon our samples
at an angle of 45○ . The focused beam size at the sample surface was
respectively.

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TABLE II. χ (2) values for each sample with different percentages of Sc concentration,
(2) (2)
where d33 = χzzz /2 and d31 = χzxx /2.

Sc (%) d33 (pm/V) d31 (pm/V)

0 5.1 ± 0.4 0.07 ± 0.006
10 15.8 ± 1.2 0.84 ± 0.05
20 42.5 ± 3.3 2.4 ± 0.1
28 46.9 ± 3.9 3.4 ± 0.2
36 62.3 ± 5.6 4.5 ± 0.3

FIG. 3. SHG measurement. (a) SHG power dependence from p-polarized input.
Black lines indicate quadratic power dependence fits for SH signal for each sam-
ple. From bottom to top, data from the 0% Sc sample are indicated by blue circles, Although d31 is much smaller than d33 , its contribution domi-
10% by orange squares, 20% by yellow diamonds, 28% by purple triangles, and nates the SH signal induced by p-polarized input light at 45 degree
36% by green crosses. (b) SH spectra from p-polarized input, similarly color coded incidence. As a result, the calculated d33 value depends strongly on
by the Sc concentration. Samples with a higher Sc concentration exhibit stronger d31 , resulting in a higher uncertainty. To better determine d33 val-
SHG. The signal from the 0% Sc sample has been scaled by a factor of 10 for
visibility.
ues in the future, a similar experiment with a larger incidence angle
would lower the effect of d31 uncertainty on d33 values.
Additionally, simulated SH power is strongly dependent on
the particular model of Pt utilized. For the analytical calculation
described in the Sec. I of the supplementary material, we utilized data
for spectral measurements. All measurements were taken under the
from Werner et al 2009.43 As our substrates are sputtered Pt, this
same conditions, accounting for sample differences like film thick-
material may not perfectly match the model, introducing additional
ness and refractive index. We confirmed the quadratic power depen-
uncertainty that cannot be accounted for in error propagation.
dence of the signal for each sample to ensure that the signal was due
to perturbative SHG, as shown in Fig. 3(a). The SHG in each sam- IV. DISCUSSION
ple exhibits p-polarization for both s- and p-polarized fundamental The χ (2) enhancement can be attributed to changes in the crystal
light, as shown in the supplementary material, Fig. 5, corroborating structure. Al1−x Scx N’s enhanced piezoelectricity is attributed to Sc
the above SHG analysis. SH spectra in Fig. 3(b) indicate significant destabilizing AlN’s wurtzite structure.25 In SHG and piezoelectric-
dependence on Sc concentration. ity, a material polarization is induced by an optical or a mechanical
The measured d33 and d31 values for all samples are shown perturbation, respectively. As such, the softened wurtzite structure
in Fig. 4 and Table II. For intrinsic AlN, we calculate d33 = 5.1
due to substitutional Sc is expected to cause a large χ (2) response as
± 0.4 pm/V and d31 = 0.07 ± 0.006 pm/V. Other experimental χ (2)
well. We expect χ (2) enhancement to continue until centrosymmetric
measurements for AlN range from 423 to 11 pm/V34 for d33 and
cubic ScN grains begin to form at Sc concentrations around 43%.25 It
smaller values ranging from 0.0423 to 0.31 pm/V for d31 .35 Thus,
is also possible that this softening in the crystal structure affects the
our calculations provide reasonable values for d33 and d31 of AlN.
For Al0.64 Sc0.36 N, we observe the largest d33 at 62.3 ± 5.6 pm/V, over relative strength of χ (2) components, with a higher Sc concentration
twice that of LN; its d31 = 4.5 ± 0.3 pm/V is also strongly enhanced inducing a lower ratio of d33 compared to d31 . Young’s or the elastic
compared to that of intrinsic AlN. modulus along the z-axis softens more quickly with the increasing
Sc concentration than that along the x-axis, indicating that the Sc
concentration affects in-plane and out-of-plane crystal axes to differ-
ent degrees.36 Furthermore, the Al1−x Scx N piezoelectric coefficients,
also written as d33 and d31 , increase at different rates with a higher
Sc concentration.36 As piezoelectric and χ (2) coefficients are simi-
larly enhanced by the softened crystal structure, it is possible that
this softening could also explain the varying ratios of d33 compared
to d31 depending on the Sc concentration. Further research should
explore the effects and determine the optimal Sc concentration
to use.
While we directly measured the second-order nonlinear opti-
cal susceptibility at optical frequencies, the enhancement from the
strained wurtzite structure could persist at lower frequencies in the
microwave regime. Since the Pockels coefficient can be expressed
in terms of χ (2) at different frequencies,31 Al1−x Scx N could exhibit
a stronger Pockels effect than intrinsic AlN, with potential applica-
tions in efficient EO modulators or integrated quantum transducers.
FIG. 4. Experimentally measured d 33 (blue diamonds) and d 31 (red circles) as It has also been found that the Sc concentration affects absorp-
functions of Sc concentration.
tion properties in the visible to ultraviolet wavelength range. While

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AlN exhibits a large 6 eV bandgap, Al1−x Scx N has a smaller bandgap, easily combine cutting-edge nonlinear technology with mature sil-
with high quality Al0.59 Sc0.41 N displaying a 4.5 eV bandgap and icon photonics and enable large-scale production of integrated non-
higher absorption at subband gap energies.33 Sample quality also linear devices, ranging from on-chip frequency converters to single-
has a significant effect, since Al0.66 Sc0.34 N was reported to have a photon sources. Future studies will improve etching processes to
bandgap of 2.94 eV.37 This was attributed to cubic ScN grain forma- produce high-quality passive photonic elements, reduce absorp-
tion at Sc concentrations as low as 20%, which could be due to the tion and waveguide loss, and produce devices including nonlinear
differences in the fabrication methods.33,37 Furthermore, AlN has a waveguides and modulators.
direct bandgap, while Al1−x Scx N’s bandgap is expected to become
indirect past concentrations of 23% Sc based on a larger measured
optical bandgap compared to theoretical predictions.33 SUPPLEMENTARY MATERIAL
Applications that utilize longer wavelengths would be min-
imally affected by the change in the bandgap. Measurements of See the supplementary material for the full derivation of abso-
Al0.85 Sc0.15 N photonic waveguides indicate losses of 9 ± 2 dB/cm lute χ (2) value, as well as additional information on ellipsometry,
at 1550 nm; however, optimizing the etching process is expected to dispersion, and birefringence. Figures of SH spectra for both input
significantly reduce sidewall roughness and loss.38 We performed polarizations, SH polarization, SEM images, and AFM images for all
prism coupling measurements of propagation loss for a wafer of samples are also included.
Al0.64 Sc0.36 N on sapphire, which indicate losses around 17.2 dB/cm
at 1550 nm, and higher loss above 30 dB/cm at 633 nm. For an
Al0.80 Sc0.20 N sample, the loss at 1550 nm is much lower, around ACKNOWLEDGMENTS
8.2 dB/cm, with loss above 30 dB/cm at 633 nm as well. Although rel- This work was funded by NSF CAREER Award No. 1944248,
atively high, these propagation loss measurements provide an upper Army Research Office (Grant No. W911NF-18-2-0048), and the
estimate of loss from absorption and may be improved by optimiz- Office of Naval Research (Grant No. N00014-20-1-2325). V.Y. is
ing grain structure. Thus, Al1−x Scx N can be used in waveguides and a recipient of the Department of Defense National Defense Sci-
other on-chip optical elements; further improvements in fabrication ence and Engineering Graduate (NDSEG) Fellowship and acknowl-
techniques could lead to reduced propagation loss. For applications edges the support from this fellowship. Fabrication and character-
at shorter wavelengths, lower Sc concentrations could enhance χ (2) ization were performed at the Singh Center for Nanotechnology at
with less effect on absorption. Further investigation is necessary to the University of Pennsylvania. Prism coupling measurements were
determine loss in Al1−x Scx N structures at different Sc concentrations performed by Metricon Corporation.
and how its absorption affects applications in different wavelength The authors and the University of Pennsylvania have U.S.
regimes. provisional patent application 63/227501 pending.
Another consideration is quasi-phase matching. While modal
phase matching can enable high performance devices, it requires
precise waveguide design and adds further constraints. Thus, many AUTHOR DECLARATIONS
devices opt instead to use ferroelectric nonlinear materials, such as
LN, which can be periodically poled to achieve quasi-phase match- Conflict of Interest
ing. While periodic poling of non-ferroelectric materials is possible The authors have no conflicts to disclose.
through doping and other fabrication techniques,39 it requires addi-
tional complicated techniques. Devices with AlN have typically used DATA AVAILABILITY
modal phase matching, but Al1−x Scx N is ferroelectric even at low Sc
concentrations,40,41 which could enable periodic poling in Al1−x Scx N The data that support the findings of this study are available
thin films. The films studied in this work were grown using identical from the corresponding author upon reasonable request.
processes to Al1−x Scx N films exhibiting ferroelectric switching with
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APL Mater. 9, 101104 (2021); doi: 10.1063/5.0061787 9, 101104-6

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