Vol. 25, No.

13 | 26 Jun 2017 | OPTICS EXPRESS 15370

Optical bandgap engineering in nonlinear

silicon nitride waveguides
C LEMENS J. K RÜCKEL , * ATTILA F ÜLÖP, Z HICHAO Y E , P ETER A.
A NDREKSON , AND V ICTOR TORRES -C OMPANY
Photonics Laboratory, Department of Microtechnology and Nanoscience, Chalmers University of
Technology, SE-412 96 Gothenburg, Sweden
* kruckel@chalmers.se

Abstract: Silicon nitride is a well-established material for photonic devices and integrated
circuits. It displays a broad transparency window spanning from the visible to the mid-IR and
waveguides can be manufactured with low losses. An absence of nonlinear multi-photon ab-
sorption in the erbium lightwave communications band has enabled various nonlinear optic
applications in the past decade. Silicon nitride is a dielectric material whose optical and mechan-
ical properties strongly depend on the deposition conditions. In particular, the optical bandgap
can be modified with the gas flow ratio during low-pressure chemical vapor deposition (LPCVD).
Here we show that this parameter can be controlled in a highly reproducible manner, providing an
approach to synthesize the nonlinear Kerr coefficient of the material. This holistic empirical study
provides relevant guidelines to optimize the properties of LPCVD silicon nitride waveguides for
nonlinear optics applications that rely on the Kerr effect.
c 2017 Optical Society of America
OCIS codes: (130.3120) Integrated optics devices; (160.4330) Nonlinear optics materials; (190.4390) Nonlinear optics,
integrated optics; (220.4241) Nanostructure fabrication.

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#290812 https://doi.org/10.1364/OE.25.015370
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1. Introduction
Silicon nitride is a well-established material in the microelectronics industry, where it has been
used as electrical and thermal insulator in electric circuits. This material can be processed
using the mature fabrication lines for electronic integration. Silicon nitride also features a set
of optical properties that makes it an ideal choice for many applications that require integration
of photonic devices on chip. Examples include ultra-high-Q resonators [1] and filters based on
ultra-low-loss waveguides [2]. Silicon nitride can also be co-integrated with active components
such as amplifiers [3], modulators and detectors [4]. The broad transparency window extends
towards the blue wavelength range, which allows for processing visible light on chip [5, 6] and
biophotonic sensing applications [7].
Another important feature of silicon nitride is that in its stoichiometric form (Si3 N4 ), it
has a nonlinear Kerr coefficient ten times higher than silica [8]. Its large optical bandgap
and high thermal damage threshold permit high optical intensities to build up in the system
without suffering from nonlinear losses in the near infrared. The potential of this material for
nonlinear optics has been demonstrated with the generation of microsesonator based frequency
combs [9–11], octave-spanning supercontinuum [12, 13] and wavelength conversion [14, 15].
The optical properties of silicon nitride depend on the conditions under which the material is
deposited. There is a wealth of empirical studies that demonstrate that varying the flow ratio of the
precursor gases during chemical vapor deposition modifies the stoichiometry of the film [16, 17].
This results in a change of refractive index, optical bandgap and film stress [16,18,19]. Increasing
the relative content of silicon vs nitride yields a silicon-rich nitride film [17]. This is highly
relevant for nonlinear optics applications because waveguides fabricated from silicon rich nitride
tend to have a higher nonlinear Kerr coefficient [20–22]. Lacava et al. recently demonstrated
that the Kerr coefficient can be enhanced by an order of magnitude in silicon nitride waveguides
fabricated via plasma-enhanced chemical vapor deposition (PECVD) by varying the silicon
content of the film [21]. However, most nonlinear optic applications are based on silicon nitride
deposited via low-pressure chemical vapor deposition (LPCVD) [9, 13, 23, 24]. Despite the
popularity of this platform, the impact of the film stoichiometry on the nonlinear properties of
LPCVD silicon nitride is not well known.
In this paper, we focus on the full characterization of the nonlinear properties of LPCVD
silicon nitride waveguides. We fabricated waveguides with five different compositions, from
stoichiometric to the maximum silicon content that is allowed in our furnace. We show that the
gas flow ratio modifies the optical properties of the material but in a highly reproducible fashion.
We present a holistic empirical study, highlighting how the gas flow ratio can be used to engineer
the optical properties of the waveguide for broadband nonlinear optic applications.
The remainder of this work is as follows. In section 2 we present the characterization of the
optical properties of the film and the waveguide fabrication process. Section 3 covers the impact
of the silicon nitride composition on waveguide propagation loss and group velocity dispersion
engineering. In section 4 we focus on the evaluation of material dependent Kerr nonlinearities
and assess the impact of waveguide confinement on the nonlinear Kerr parameter. In section 5
we compare the measured Kerr nonlinear coefficients with theoretical expectations and establish
a comparison between LPCVD and PECVD silicon nitrides as well as other material platforms
used for nonlinear optic applications.
 Vol. 25, No. 13 | 26 Jun 2017 | OPTICS EXPRESS 15373

2. Fabrication and material properties

We fabricated high-confinement strip waveguides with a silicon nitride core surrounded by a
silicon dioxide cladding. For the deposition of silicon nitride (SiN), we used dichlorosilane
(DCS) and ammonia (NH3 ) as precursor gases in an LPCVD furnace (Centrotherm). In order to
form the waveguide core, the SiN film was patterned by optical contact lithography (DUV) and
dry etching (CHF3 +O2 ). The process steps were similar to the ones presented in [20] and further
advanced by including a standard cleaning step after etching.
Throughout the fabrication and characterization process, it became clear that the ratio between
the two precursor gases DCS and NH3 is the most relevant parameter to control the properties of
the SiN film. The ratio DCS:NH3 directly impacts the atomic composition of the material. It
yields an increase in silicon content with increased gas ratio [16]. We have confirmed this trend
with measurements based on X-ray diffraction [20]. Throughout this paper we will however use
the ratio DCS:NH3 to describe the composition because it provides a more accurate means to
control the fabrication process. The relation between gas flow ratio and atomic composition in
LPCVD SiN has been reported in the literature [16].
We fabricated five different SiN compositions. The chosen gas ratios DCS:NH3 reached from
0.3 for stoichiometric silicon nitride (Si3 N4 ) to non-stoichiometric silicon nitride (Six Ny ) with
a maximum gas ratio of 16.7 given by the gas flow limits of the furnace. For deposition of
Si3 N4 we used the recipe provided by Centrotherm. All films were deposited under similar
temperature conditions around 800◦ C and the pressure was optimized to reach both stable
deposition conditions and best possible film uniformity.
The target height and width of the fabricated waveguide core were 700 by 1650 nm for all
compositions. Stoichiometric Si3 N4 films display cracks at this thickness, so we etched crack
barriers following a similar process to [25, 26] into the bottom oxide using a laser writer tool
followed by a wet-etch step in order to minimize waveguide imperfections. The patterned
structures increased the crack-free area of the wafer to several cm2 as cracks originating from
wafer handling were stopped. However, full control of cracks was not achieved. Etching into the
silicon substrate was suggested in [27] to get rid of this issue. It is worth emphasizing that films
deposited using gas ratios above ∼4 had no cracks at the fabricated thickness of 700 nm owing to
a decrease in stress for silicon-rich nitride. As an example, the measured stress in stoichiometric
Si3 N4 films (DCS:NH3 0.3) lied above 1200 MPa whereas films from DCS:NH3 12 had values
around ∼500 MPa.
We used spectroscopic ellipsometry for the analysis of the refractive index properties of the
materials. We fitted the measurement data using a Tauc-Lorentz oscillator model [28]. This
model yields the resonance pole information and optical bandgap. Figure 1(a) shows the real
part of the refractive index for all fabricated compositions within the wavelength range of the
ellipsometer (245-1000 nm) and the extrapolation up to 2000 nm. One can observe that, at a
fixed wavelength, the refractive index increases with higher gas flow ratio. This is consistent
with an increase of silicon content in the film [16]. Figure 1(b) illustrates the variation of the
optical bandgap of the material with the gas flow ratio. It is clear that by increasing the gas flow
ratio, the optical bandgap of the film decreases, but it always remains above the energy level for
two-photon absorption to take place at 1550 nm, as indicated by the dotted red line. Physically
the measured optical bandgap corresponds to the photon energy at which the imaginary part of
the refractive index, k, becomes non-zero, as shown in the figure inset. The absence of material
loss for wavelengths above 350–600 nm clearly indicates the ultra-broad transparency window
of silicon nitride.
We studied the uniformity of the SiN films by realizing repeated ellipsometer area scans. The
uniformity was measured with 137 points across the 3-inch wafer with an x-y-position change of
0.5 cm. For illustration purposes we used a SiN film fabricated with the gas ratio 8 in Fig. 1(c),
but similar results were obtained for the other compositions and over independent fabrication
 Vol. 25, No. 13 | 26 Jun 2017 | OPTICS EXPRESS 15374

2.6 3.5 0.02

Si3N4 - DCS:NH3 0.3
2.5 SixNy - DCS:NH3 4 0.01
SixNy - DCS:NH3 8
3

k
2.4 SixNy - DCS:NH3 12
refractive index

bandgap [eV]
SixNy - DCS:NH3 16.7 0

2.3
-0.01
2.5 300 350 400 450 500 550 600 650
2.2 wavelength [nm]

2.1
2
2 TPA limit @1550 nm

1.9 1.5
200 500 1000 1500 2000 0 5 10 15 20
wavelength [nm] gas ratio DCS:NH3
(a) thickness [nm] (b)
720
-3 0.2
deviation per wafer

deviation [%] (@ 850 nm)

715
-2 deviation per run
y-position [cm]

0.15
refractive index
710
-1
0 705
0.1
1 700

2 695 0.05

3 690
0
0 5 10 15 20
-3 -2 -1 0 1 2 3
gas ratio DCS:NH3
x-position [cm]
(c) (d)

Fig. 1. (a) Measured refractive index as a function of wavelength for different SiN compo-
sitions. The shadowed area shows extrapolated data from the measurements. (b) Optical
bandgap as a function of gas flow ratio. The two-photon absorption limit indicates twice the
photon energy at 1550 nm wavelength. The inset shows a zoomed in part of the measured
imaginary refractive index k as a function of wavelength for the fabricated compositions. (c)
Area scan of the film thickness with 139 points showing the uniformity of the deposited SiN
film on a 3-inch wafer (DCS:NH3 8). (d) Reproducibility of the refractive index at 850 nm
carried out over 22 points on a single wafer and between 3 independent deposition runs.

runs. A maximum deviation from target (700 nm) below 3% can be observed. Such non-local
change in film height should be considered when designing waveguide dimensions for dispersion
engineering. Next, we studied the reproducibility of the film composition by first comparing the
refractive index change across a single wafer (22 measurement points) and second by comparing
the average refractive index of 3 wafers from independent deposition runs. The results are shown
in Fig. 1(d). A deviation below 0.15% is reached in both cases when measuring ∼200 nm thick
films. Thin films were chosen here to reduce processing time. This study shows that the gas
flow ratio in an LCPVD furnace provides a reliable way to control the optical properties and
composition of the SiN films.
 Vol. 25, No. 13 | 26 Jun 2017 | OPTICS EXPRESS 15375

3. Linear waveguide properties

3.1. Waveguide propagation loss
We evaluated waveguide propagation losses and coupling losses using the cut-back method with
3 different lengths. The loss measurements were done in a spectrally resolved manner from 1510
to 1610 nm and the polarization was optimized for maximum system throughput. In order to
present representative data, we performed the measurements over 5 waveguides. The averaged
values and standard deviation per wavelength are presented in Fig. 2. Changes in propagation
losses for the different compositions are expected to originate from material properties of the
SiN waveguide core and from a variation of the modal interaction at the core-cladding interfaces
due to composition specific waveguide confinement.
For the waveguides with gas flow ratio 4 to 16.7 the three cut-back lengths were 4, 3 and
1 cm. The waveguides fabricated from Si3 N4 had lengths of 2.2, 1.3 and 0.9 cm because we
had to restrict ourselves to the crack-free area of the wafer. Instead of the straight waveguides
used in this work, a space saving design (spiral, meander) is recommended if film cracks cannot
be avoided. We used horizontal coupling directly into the waveguide core via tapered lensed
fibers with 2.5 µm spot size diameter. Coupling losses ∼4 dB per facet were obtained for all
compositions. The larger uncertainty in the Si3 N4 waveguide losses is due to the shorter cut-back
lengths, resulting in lower measurement precision. We observe a reduction in waveguide loss
with decreasing gas flow ratio. The typical absorption resonance around 1.53 µm is visible for
all compositions with DCS:NH3 ≥4. This is likely due to the existence of N-H bonds that remain
from the use of ammonia as precursor gas. This fact alone however cannot explain the increase
absorption observed in the L band. Interestingly, we could get rid of the absorption resonance
for DCS:NH3 0.3 by realizing an annealing step at 1200◦ C over 3 h in nitrogen atmosphere.
The final losses after annealing for Si3 N4 were around 0.4 dB/cm at 1550 nm wavelength,
a value comparable to other reported values in the literature using waveguides with similar
dimensions [13]. We estimate the scattering losses contribute 0.2 dB/cm [20]. Additional steps,
such as the use of a higher quality LPCVD top oxide layer could further improve the propagation
losses [27]. How well the annealing step can be applied to the other composition requires further
investigations. For example the same annealing recipe caused an increase in waveguide loss
for the silicon-rich composition DCS:NH3 8. We suggest that the losses are caused by the
formation of silicon clusters, since a similar effect has been reported in the literature when
annealing silicon-rich nitride films [29]. Whether the losses of the silicon-rich nitride films can
be decreased with a different annealing recipe deserves further investigation because, as we shall

10 10 10 10 10
DCS:NH 3 16.7 DCS:NH 3 12 DCS:NH 3 8 DCS:NH 3 4 DCS:NH 3 0.3
waveguide loss [dB/cm]

8 8 8 8 8
0.7 µm
6 6 6 6 6
1.65 µm

4 4 4 4 4
loss@1550 nm loss@1550 nm loss@1550 nm loss@1550 nm loss@1550 nm
~7.3 dB/cm ~4.4 dB/cm ~1.4 dB/cm ~1.4 dB/cm ~0.4 dB/cm
2 2 2 2 2
1 1 1 1 1
0 0 0 0 0
1510 1560 1610 1510 1560 1610 1510 1560 1610 1510 1560 1610 1510 1560 1610
wavelength [nm] wavelength [nm] wavelength [nm] wavelength [nm] wavelength [nm]

Fig. 2. Waveguide propagation loss as a function of wavelength for waveguides with 5

different silicon nitride compositions corresponding to different DCS:NH3 ratios. The darker
colored line shows the mean value and the brighter shadowed areas illustrates the standard
deviation of the loss measurements. The inset shows the waveguide core after etching.
 Vol. 25, No. 13 | 26 Jun 2017 | OPTICS EXPRESS 15376

show in the next section, these materials display very high nonlinear Kerr coefficient.

3.2. Numerical analysis of waveguide dispersion

Here we look into the dispersion engineering possibilities of the SiN waveguides. The waveguide
dispersion can be engineered over a broad wavelength range by tailoring its dimensions [30] or
in the case of a silicon nitride waveguide by changing its material composition [31].
The simulations were performed with a modesolver based on COMSOL-Multiphysics us-
ing the refractive index data for the core and cladding materials extracted from ellipsometer
measurements. First, we show how the waveguide width and height individually impact the group
velocity dispersion profile β2 . This is exemplified in Fig. 3(a) for the SiN composition fabricated
using the gas ratio 16.7 for the fundamental quasi TE-mode. The left illustration shows that an
increase in waveguide height is required (fixed width of 1.65 µm) in order to reach anomalous
GVD. In the right illustration it can be seen that varying the waveguide width allows to shift the
second zero dispersion wavelength to lower optical frequencies.
The impact of both waveguide width and height together is studied in Fig. 3(b) in more detail.
Here, we show how the GVD changes for all geometry combinations for a width from 0.4 to

400 400
width 1.65 µm, height 0.5 µm height 0.7 µm, width 1.05 µm
width 1.65 µm, height 0.6 µm height 0.7 µm, width 1.35 µm
β2 [ps2 /km]

β2 [ps2/km]

width 1.65 µm, height 0.7 µm height 0.7 µm, width 1.65 µm
200 200

0 0

-200 -200
1000 1200 1400 1600 1800 2000 2200 2400 1000 1200 1400 1600 1800 2000 2200 2400
wavelength [nm] wavelength [nm]
(a)
β 2 [ps2/km] 2
2 DCS:NH3 0.3
DCS:NH 3 16.7 400 DCS:NH3 4
1.8 1.8
DCS:NH3 8
350 DCS:NH3 12 anomalous
1.6 1.6
300 DCS:NH3 16.7
GVD
width [µm]

width [µm]

1.4 1.4
250
anomalous GVD
1.2 200 1.2
1 normal GVD 150 1
100 normal GVD
0.8 0.8
50
0.6 0.6
0
0.4 0.4
0.3 0.4 0.5 0.6 0.7 0.8 0.9 1 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1
height [µm] height [µm]
(b) (c)

Fig. 3. (a) Impact of height and width variation on the group velocity dispersion (DCS:NH3
16.7, quasi-TE-mode). (b) Group velocity dispersion coefficient β2 as a function of waveg-
uide width and height of the silicon nitride waveguide considering the material corresponding
to DCS:NH3 16.7 (1550 nm wavelength, quasi-TE-mode). The black line indicates the di-
mensions at which zero GVD occurs. The circle indicates the dimensions of the fabricated
waveguides. (c) Waveguide dimensions at which crossing from normal to anomalous disper-
sion occurs (1550 nm wavelength, quasi-TE-mode). The circle indicates the dimensions of
the fabricated waveguides.
 Vol. 25, No. 13 | 26 Jun 2017 | OPTICS EXPRESS 15377

2 µm and a height from 0.25 to 1 µm. This allows relating the dispersion profile to the optical
confinement. The illustration is valid for the fundamental quasi-TE-mode at wavelength of 1550
nm. Waveguide dimensions that lead to β2 values of zero are lying along the black line. Thus,
anomalous dispersion is achieved for the dimensions on the right side of this line. We compared
the dimensions required to cross from normal to anomalous dispersion for all fabricated SiN
compositions, see Fig. 3(c). The larger refractive index of the silicon rich compositions causes
in general a shift of the anomalous GVD crossing towards thinner and narrower dimensions.
This trend is expected, since a higher silicon rich composition provides higher refractive index
contrast and allows for higher mode confinement in the core. This result will be further discussed
in the next subsection in the context of optimization of the nonlinear parameter. It can be seen that
for the fabricated dimensions, anomalous dispersion at 1550 nm is achieved for all compositions
except for Si3 N4 .

4. Nonlinear properties
In this section we illustrate that the nonlinear Kerr coefficient of silicon nitride strongly depends
on the gas flow ratio utilized during deposition. First, we evaluate the nonlinear parameter γ
in measurements based on a dual-pump experiment [20, 32] where the nonlinear phase shift is
measured as a function of optical pump power, i.e. θnl = γPL eff , with L eff being the effective
length of the waveguide. The measurements were carried out around 1563 nm. This experiment
also served as a means to verify the absence of multi-photon absorption at telecom wavelengths
up to several hundreds of mW continuous-wave (CW) pump power coupled into the waveguide.
The slope in the linear fit of θnl vs P provides an estimation of the nonlinear parameter γ of
the waveguide with knowledge of L eff . The results of the measurements are summarized in Fig.
4(a) by the circular symbols. The calculation of the errors includes both the error in the slope
and the error in L eff provided by the uncertainty in the losses (Fig. 2). It is clear that increasing
the flow ratio yields a higher nonlinear parameter. This however does not necessarily mean
that the nonlinear Kerr coefficient increases. To verify this, we calculated the Kerr coefficient
as n2 = γλ Aeff /2π. The effective area can change even if the cross-section is identical for

12 0.9 1.3
dimension - fabricated
11 dimension - max γ + zero GVD SiN 0.7 µm 1.2
10 dimension - max γ 0.875 1.1
1.65 µm SiO 2
9 1
m /W]

8 0.85 0.9
γ [(W.m)-1 ]

Aeff [ µm2 ]

0.8
2

7
0.825 0.7
-18

6
0.6
n2 [·10

5 0.5
4 0.8
0.4
3 0.3
2 0.775 0.2
1 0.1
0.75 0
0 0 5 10 15 20 0 5 10 15 20
0 5 10 15 20
gas ratio DCS:NH3 gas ratio DCS:NH3 gas ratio DCS:NH3
(a) (b) (c)
Fig. 4. (a) Circles - Measured nonlinear parameter γ with the fabricated dimensions (0.7 µm
height and 1.65 µm width). Diamonds - Numerical simulations of the maximum γ at the
dimensions that give the highest optical confinement in the waveguide. Squares - Numerical
simulations of the largest achievable γ with the restriction to have zero group-velocity
dispersion. (b) Simulation results of the effective area Aeff for the fabrication gas ratios.
(c) Evaluated nonlinear Kerr coefficient from the measured nonlinear parameter γ and the
simulated effective area Aeff .
 Vol. 25, No. 13 | 26 Jun 2017 | OPTICS EXPRESS 15378

all compositions. This fact is illustrated in Fig. 4(b). The effective area decreases for larger
DCS:NH3 ratios, which results from the higher optical confinement owing to the increase in
refractive index. Figure 4(c) shows the estimated n2 for each of the measured SiN compositions.
It is clear that the Kerr coefficient can be modified by roughly a factor of 4 by controlling the gas
flow ratio during film deposition; from n2 = (0.31 ± 0.04) · 10 −18 m2 /W for Si3 N4 (DCS:NH3
0.3) to n2 = (1.13 ± 0.13) · 10 −18 m2 /W for DCS:NH3 16.7.
The results in Fig. 4(a) (circles) correspond to the nonlinear Kerr parameter measured for
different compositions with identical cross-section. This parameter could be further enhanced by
optimizing the waveguide dimensions for each composition. This is illustrated in Fig. 5(a) using
the composition corresponding to DCS:NH3 16.7. The parameter γ is maximized for a waveg-
uide whose dimensions provide the highest optical confinement. The dimensions correspond
to 0.82 µm width and 0.4 µm height (highlighted by the diamond symbol in Fig. 5(a)). This
maximum value is almost double the value we measured for the fabricated geometry. However,
comparing this plot with Fig. 3(b), it becomes clear that this cross-section geometry does not
yield anomalous dispersion. This conclusion is generally valid for all compositions. One could
instead calculate the geometry that provides the maximum nonlinear parameter within the zero
GVD contour in Fig. 3(b) (plotted again in Fig. 5(a)). This point is defined by the square symbol
in Fig. 5(a). This analysis is carried out for all compositions and the results are presented in Fig.
4(a), where the measured nonlinear parameter for each composition is compared to what could
be obtained if the waveguide dimensions were optimized. The nonlinear parameter could be
enhanced by almost an order of magnitude by varying the stoichiometry of the film with respect
to the measured value in stoichiometric silicon nitride.
Of course, the relevant parameter for most nonlinear optics applications in absence of multi-
photon absorption is the amount of nonlinear phase shift per unit power, i.e. θnl /P = γL eff . This
figure of merit is important, as the nonlinear parameter alone does not provide the whole picture.

γ [(W . m)-1] 0.25

2 10
dimension - fabricated DCS:NH 3 16.7
dimension - max γ + zero GVD
1.8 dimension - max γ 9
0.2
1.6 8
γ · max Leff [rad/W]

1.4 7
width [µm]

0.15
6
1.2
5 0.1
1
4
0.8
3 0.05
0.6 2
0.4 0
0.3 0.4 0.5 0.6 0.7 0.8 0.9 1 0 5 10 15 20
height [ µm] gas ratio DCS:NH3
(a) (b)

Fig. 5. (a) Nonlinear parameter for different width and height of the waveguide core fab-
ricated from DCS:NH3 ratio 16.7. The simulations are made for the fundamental quasi
TE-mode at 1550 nm wavelength. The plot indicates the fabricated waveguide dimensions,
the dimensions that lead to a maximum nonlinear parameter, and the dimensions that result in
a maximum nonlinear parameter with the requirement of zero GVD. (b) Maximum relative
nonlinear phase shift γ · max L eff achieved for the fabricated waveguide dimensions of 700
nm height and 1650 nm width.
 Vol. 25, No. 13 | 26 Jun 2017 | OPTICS EXPRESS 15379

In order to include propagation losses, we considered the case of maximum achievable effective
length, max L eff , as 1/α with α being the linear loss. The results for our materials are shown
in Fig. 5(b). Surprisingly, the plot indicates two optimum compositions that yield maximum
nonlinear phase shift. Composition DCS:NH3 0.3 is stoichiometric silicon nitride and it benefits
from very low propagation losses. Composition DCS:NH3 8 corresponds to the results previously
reported in [20, 33]. This material reaches a similar nonlinear phase shift due to its increased
nonlinear coefficient and moderate linear loss. The large uncertainty in the standard deviation for
the Si3 N4 material comes from the high uncertainty of the low waveguide losses, which has a
larger impact when calculating max L eff . It is important to emphasize that this comparison is
not fundamental. Further decrease in propagation losses for one or another composition could
dramatically change this picture.

5. Theoretical comparison and discussion

In order to understand the fundamental limitations of the Kerr effect in our platform and to validate
our experimental results, we compare our measured values of the nonlinear Kerr coefficient n2
with theoretical expectations. A useful theoretical approach developed by Sheik-Bahae et al. [34]
links n2 directly to the optical bandgap of the material according to
G2 (~ω/Eg )
n2 = K 0 . (1)
n02 Eg4

This equation is developed under the assumption that there is a Kramers-Kronig relation between
the real and imaginary parts of the nonlinear refractive index and that the nonlinear absorption
is dominated by two-photon absorption [34]. The relation is valid for a broad range of photon
frequencies, even when they are far below the optical bandgap. This is taken into account by
the function G2 . In the equation above, n0 is the refractive index and K 0 is a constant. The
function G2 is maximized for photon energies close to Eg /2 thus suggesting that highest Kerr
nonlinearities are attained when using a wavelength close to the TPA limit. The formulation is
valid for solids provided the assumptions above hold. In such case, it gives reasonable estimates
for a broad range of oxides and glasses [35].
Figure 6 indicates that the properties of our materials follow reasonably well the Sheik-Bahae
relationship. The photon energy and refractive index were taken at 1563 nm, the wavelength of the
dual-pump experiment. Uncertainties from the Kerr coefficient evaluation are not considered here.
For comparison, other widely used nonlinear materials are included in Fig. 6 based on data of

0 a-Si:H Si3N4 - DCS:NH3 0.3

10
PECVD Si 7 N 3 6
SixNy - DCS:NH3 4
n2n02 /(K’G2) [m2/W]

SixNy - DCS:NH3 8
-1 c-Si
10 SixNy - DCS:NH3 12
SixNy - DCS:NH3 16.7
-2
10 PECVD Si 3 N 4
LPCVD Si x N y
LPCVD Si 3 N 4
-3
10 SiO 2
This work
-4 References
10
1 2 3 4 5 6 7 8 9 10
Eg [eV]

Fig. 6. Rescaled nonlinear Kerr coefficient as a function of optical bandgap. The blue line
indicates the 1/Eg4 relation. See text for more details.
 Vol. 25, No. 13 | 26 Jun 2017 | OPTICS EXPRESS 15380

refractive index, nonlinear Kerr coefficient and bandgap provided in the references. The way the
bandgap is defined is not explicitly mentioned in the publications. This may lead to a discrepancy
in Eg . At the two extremes of the bandgap scale, we find crystalline silicon (c-Si) [36, 37]
and silicon dioxide (SiO2 ) [38, 39]. These materials display different Kerr nonlinearities in
comparison to our silicon nitride compositions but they follow qualitatively the scaling 1/Eg4 .
It is interesting to note that the two low bandgap materials deposited with PECVD, namely
hydrogenated amorphous silicon (a-Si:H) [40, 41] (refractive index of 3.5 was assumed) and
Si7 N3 [22] display a huge increase in nonlinearities but a significant deviation from the Sheik-
Bahae relation. Our LPCVD Si3 N4 display a Kerr coefficient value [n2 = (0.31 ± 0.04) · 10 −18
m2 /W] in agreement with previously reported values in the literature [42]. This value is also
compatible with the value reported for PECVD Si3 N4 [8, 43].

6. Conclusion
We have demonstrated that the gas flow ratio in the LPCVD process to synthesize silicon nitride
can be used to control the nonlinear characteristics of an integrated waveguide. Essentially, the
gas flow ratio modifies the frequency location of the optical bandgap, which in turn varies the
refractive index and Kerr coefficient. These parameters increase with higher gas flow ratios. We
did not observe nonlinear absorption in the erbium telecommunications band up to hundreds of
mW of optical power coupled into the waveguide. The nonlinear Kerr coefficient of LPCVD
silicon-rich nitride follows qualitatively a Sheik-Bahae relationship. We found two compositions
yielding an optimum nonlinear phase shift per launched power, one was stoichiometric silicon
nitride (Si3 N4 ) and the other one a composition with slightly increased silicon content [20]. The
performance of the former is due to the relatively low linear losses, whereas the latter provides an
increase in nonlinear parameter. The possibility to modify the refractive index of the waveguides
in a highly reproducible fashion opens up a new way to engineer the dispersion of silicon nitride
waveguides and enhance their nonlinear characteristics.

Funding
This work was supported by the European Council under grant agreement ERC-2011-AdG-
291618 PSOPA, the Wallenberg Foundation and the Swedish Research Council (VR).