LASER
& PHOTONICS
Laser Photonics Rev., 1–19 (2016) / DOI 10.1002/lpor.201600038
Abstract We review the progress in the development of fre-
quency converters based on three-wave mixing in whispering
gallery resonators (WGRs). The theoretical description, given
in a unified notation for all basic processes, reveals that the
phase-matching condition known from conventional devices is
replaced by several selection rules and, furthermore, the fact
that conversion efficiencies of more than 25% can be reached
in the overcoupled regime only. Experimentally, the conversion
efficiencies exceed 50% already at milliwatt input powers. This is
achieved, however, so far in bulk resonators only since today the
on-chip devices have two orders of magnitude lower quality fac-
tors. Regarding the stability of the conversion process, one has
to consider impurities left from the crystal growth and material
Three-wave mixing in whispering gallery resonators
Ingo Breunig∗
1. Introduction
Optical frequency converters based on three-wave mixing,
i.e. on second-order nonlinear effects, are nowadays work-
ing horses in science and in industrial applications. We
find harmonic generators in almost every laser laboratory
and in laser machining facilities. Optical parametric oscilla-
tors (OPOs) emit pulsed and continuous-wave light tunable
from the visible to the far-infrared [1–3]. Highly sensi-
tive infrared cameras are based on sum-frequency mixers
[4]. Finally, difference-frequency mixers are utilized for the
generation of laser light in the mid- and far-infrared spectral
range [5].
In order to increase the conversion efficiency, three-
wave mixers typically comprise a suitable mirror resonator
enhancing the power of the circulating light by orders of
magnitude. The integration of these devices on centimeter-
sized chips was achieved by using waveguiding structures
having reflective coatings at the end facets [6]. However,
miniaturization into the sub-millimeter range as it is known
from laser diodes is challenging. The efficiency is weaker
for smaller devices because of shorter interaction lengths.
This has to be compensated by coatings highly reflecting
two or even three of the interacting waves. Taking into
account that the respective wavelengths are considerably
different, this can be pretty sophisticated.
In 2004 this unsatisfactory situation has changed: A
team from the Jet Propulsion Laboratory in the United
States has presented a frequency doubler based on an op-
tical whispering gallery resonator (WGR) [7]. Here, the
circulating light is guided by total internal reflection in
monolithic spheroidally-shaped dielectric. Consequently,
these cavities provide perfect reflectivity over the entire
transparency range of the material without any coating.
University of Freiburg, Department of Microsystems Engineering (IMTEK), Georges-Köhler-Allee 102, 79110 Freiburg
∗
Corresponding author: e-mail: ingo.breunig@imtek.de
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specific effects like photoconductivity, photorefractivity, and py-
roelectricity. The impressive experimental progress paves the
way that micrometer-sized frequency converters based on
WGRs will find the way out of the lab into real-world applications.
Furthermore, micrometer-scaled whispering gallery res-
onators can be easily integrated into chips [8].
Since the pioneering first demonstration of second-
harmonic generation in a WGR, there has been a tremen-
dous development in the field of WGR-based three-wave
mixing. All basic processes have been modeled theoreti-
cally using different approaches and diverse notations. In
experiments, millimeter-sized WGRs made of bulk crys-
tals were employed as well as micrometer-sized devices
integrated on chips.
Several reviews on whispering gallery resonators in
general have been published before [9–13]. Some more
review articles concentrate on specific applications like
lasing [14, 15], sensing [16], cavity optomechanics [17],
or second-harmonic generation [18]. In this article, an
overview of the evolution of frequency conversion in WGRs
based on the second-order nonlinearity, i.e. three-wave mix-
ing, during the last decade is given. We summarize the re-
sults of different theoretical models in a unified notation
for all basic processes. Different fabrication techniques and
experimental achievements are discussed comparing those
of bulk resonators with the ones of on-chip devices. We will
consider material limitations and, finally, discuss the per-
spectives of whispering-gallery-resonator-based frequency
converters.
2. Theoretical considerations
For a strong second-order nonlinear-optical interaction, the
three light fields involved have to exhibit a large spatial
overlap and to fulfill the phase matching condition. Fur-
thermore, the efficiency of resonator-enhanced three-wave
mixing depends on how much light is coupled into and out

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2 I. Breunig: Three-wave mixing in whispering gallery resonators
Figure 1 a) Spheroidal shape given by the radii R and ρ and
coordinates u, ϕ, and ϑ. Normalized eigenfunctions m,p,q for
R = 1 mm and ρ = 0.25 mm. b) 60,2,1 in the equatorial and
polar planes. c) 10000,p,q , p = 0 . . . 2, q = 1, 2 in the polar plane
(ϕ = 0). The scale bar measures 10 × 10 µm2 .
of the cavity. Thus, in the next two sections, we will iden-
tify the spatial field distributions - the whispering gallery
modes - and the corresponding values for the resonant fre-
quencies and propagation constants followed by consider-
ations about coupling in and out. Then we will put these
basic ingredients together with the coupled mode equations
for three-wave mixing in order to derive explicit expres-
sions for the efficiencies of different frequency conversion
processes.
2.1. Whispering gallery modes
Most of the whispering gallery resonators applied for three-
wave mixing so far exhibit a mm-sized spheroidal shape
determined by the major and minor radii R and ρ (see
Fig. 1a). Since the light propagates at the rim close to the
equator of the cavity, we employ a curvilinear coordinate
system with the azimuth angle ϕ, the polar angle ϑ and the
distance u from the rim. We restrict our analysis to light
fields located close to the equator (u  ρ and ϑ  1).
The general idea behind this approximation is described in
[19]. It leads to an expression for the spatial electric-field
distribution m, p,q , which is characterized by the mode
numbers m, p and q. Specifically, we find [20]:
 
m, p,q ∝ Ai u/u m + αq × e−ϑ /2ϑm H p (ϑ/ϑm ) × cos(mϕ)
2 2
(1)
with u m = 2−1/3 m −2/3 R and ϑm = (R/ρ)3/4 m −1/2 . Here,
αq < 0 are the q th zeros of the Airy function and H p the
p th -order Hermite polynomials.

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The basic spatial structure of , displayed in Figs. 1b,c,
is described by the azimuthal mode number m (oscillations
in ϕ direction), the polar mode number p (zeros in ϑ direc-
tion) and the radial mode number q (extrema in u direction).
For visible or near-infrared waves propagating in a mm-
sized whispering gallery resonator m is about 104 . Their
cross section measures ∼ 100 µm2 and their mode volume
is approximately 106 µm3 . Another important feature is re-
lated to the symmetry of the electric-field distribution.  is
antisymmetric with respect to the equatorial plane for odd
values of p and symmetric for even ones. This is of great
importance for three-wave mixing since it leads to selection
rules as it will be discussed below in more detail.
The electric-field distributions m, p,q correspond to the
resonant frequencies [20]
 √ 
mc0 αq (2 p + 1) R
νm, p,q  1 − 1/3 2/3 + √
2π Rn 2 m 2m ρ
mc0
≡ (2)
2π Rn eff
with the vacuum speed of light c0 , the bulk refractive in-
dex n and the effective refractive index n eff < n. From
this expression, we can determine the effective propagation
constant
2π νm, p,q m
keff = n eff = . (3)
c0 R
The discretization of the propagation constant converts the
continuous phase matching condition for three-wave mix-
ing processes into a simple selection rule. This will also be
discussed below in more detail.
Equations (1) and (2) are valid if the evanescent field
outside of the resonator can be neglected, thus for m 
100. For optical waves propagating in a mm-sized WGR,
the accuracy can be considered as very high. Analytical
expressions with higher order corrections comprising also
a polarization dependence are given in [21–23]. Recently,
they have been successfully applied for the determination
of the mode numbers from a fit to the resonance spectrum of
a mm-sized resonator[24]. For WGRs having a shape that
deviates from a sphere or a spheroid, numerical simulations
as described in [25] can be applied in order to characterize
the whispering gallery modes.
2.2. Coupling in and out
Coupling light into and out of a whispering gallery resonator
is commonly achieved by frustrated total internal reflection.
For the theoretical modeling, it is very instructive to leave
aside specific details of the coupler (prism, tapered fiber,
etc.) and to apply a general approach as it was done in
[26, 27]. The coupler can be represented by a 2 × 2 matrix
with the real transmission and coupling coefficients t and
κ such that κ 2 + t 2 = 1 (see Fig. 2). This matrix links the
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Laser Photonics Rev. (2016)
Figure 2 Resonator with major radius R and coupler described
by the coefficients t and κ. Its input and output amplitudes are
aA,B and bA,B .
input and output amplitudes as
     of the WGR as well as how much light can be coupled into
aB t κ aA
= . (4)
bA −κ t bB
Here, aA,B represent the complex amplitudes of the light
fields outside the resonator and bA,B the internal ones. They
are normalized in such a way that their squared absolute
value gives the respective optical power. It should be noted
that, in general, κ and t are complex since they have to
account for phase jumps at the coupling point. Since our
goal is to obtain relations for output powers instead of
fields, we are free in the choice of the phase jumps as
long as we fulfill the energy conservation |aB |2 + |bA |2 =
|aA |2 + |bB |2 .
On its path along the rim of the resonator with the cir-
cumference L = 2π R, part of the light field is absorbed by
the material. We can write bB = exp(−αL/2) exp(iδφ)bA
using the absorption coefficient α and the phase shift δφ in
order to take non-resonance into account. Combining this
expression with Eq. (4) and assuming a small propagation
loss as well as a small deviation from resonance we get for
the coupling efficiency [28]
|aB |2 4r
K ≡1− = (5)
|aA | 2 4(δν/ ν0 )2 + (1 + r )2
with the ratio r = κ 2 /αL between coupling and internal
loss, the deviation δν = (c0 /2π Ln)δφ from a resonance
frequency, and the intrinsic linewidth ν0 = c0 α/2π n. The
function K (δν) has a lorentzian shape with the maximum
K res = 4r/(1 + r )2 at resonance and the full width ν =
ν0 (1 + r ) at half maximum (see Fig. 3). Thus, the quality
factor of the whispering gallery resonator is given by Q ≡
ν/ ν = Q 0 /(1 + r ) with the intrinsic quality factor Q 0 =
ν/ ν0 = 2π νn/c0 α.
Figure 3 shows how K res and Q/Q 0 depend on the
coupling ratio r . For strong undercoupling (r  1) the in-
trinsic loss is the major contribution to the quality factor,
while it can be neglected for strong overcoupling (r 1).
At critical coupling (r = 1) the coupling efficiency reaches
unity. Obviously, the ratio r determines the quality factor
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Figure 3 Left: Coupling efficiency K as a function of frequency
detuning δν for ν0 = 3 MHz and r = 2 according to Eq. (5) with
the maximum Kres at resonance and the linewidth ν. Right:
Coupling efficiency Kres and ratio Q/Q0 between total and intrinsic
quality factor as a function of r .
the cavity. Below, we will see that it is a crucial parameter
for the optimization of nonlinear-optical three-wave mixing
too.
The generic approach used above does not include
details about the coupler. Thus, the coefficient κ 2 is not
linked with experimental parameters. In Ref. [28], κ 2 is
discussed for three different kinds of couplers: fibers, slab
waveguides, and prisms. For all of them the √ relation r ∝
κ 2 = C exp(−2γ D) holds with γ = (2π ν/c0 ) n 2 − 1 and
the distance D between coupler and resonator. Thus, κ 2
and consequently the ratio r are maximized if the coupler
touches the resonator. The constant C determining the upper
limit of r strongly depends on which coupler is employed,
on the resonator radii, on the wavelength, etc. It varies over
several orders of magnitude.
In this article, we restrict our argumentation on a simple
scheme with a single coupler since it is employed in most
experiments. However, it can be advantageous for some
applications to utilize add/drop ports. In order to take such
a scheme into account, one has to add more couplers.
2.3. Nonlinear-optical three-wave mixing
2.3.1. General considerations and selection rules
For the theoretical description of nonlinear-optical pro-
cesses, we consider three interacting waves with the respec-
tive frequencies ν1,2,3 such that ν1 + ν2 = ν3 propagating
along the z direction. The classical coupled wave equations
[29, 30] commonly used to describe bulk devices read
d α1 2π ν1 d
E1 = − E1 − i E 3 E 2∗ e−i kz
dz 2 c0 n 1
d α2 2π ν2 d
E2 = − E2 − i E 3 E 1∗ e−i kz
dz 2 c0 n 2
d α3 2π ν3 d
E3 = − E3 − i E 1 E 2 ei kz
(6)
dz 2 c0 n 3

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4 I. Breunig: Three-wave mixing in whispering gallery resonators
Figure 4 Three waves with the normalized amplitudes bi (z)
propagate along the rim. Each of them has a certain spatial in-
tensity profile given by i2 (x, y ).
with the complex slowly varying amplitudes E i , the inten-
sity absorption coefficients αi , the refractive indices n i , and
the nonlinear-optical coefficient d. The phase mismatch
k = k3 − k2 − k1 comprises the propagation constants
ki = 2π νi n i /c0 . In this form, the set (6) is not useful for
the description of three-wave mixing processes in whisper-
ing gallery resonators sketched in Fig. 4. We need to take
into account the transverse mode structure given by Eq. (1)
as well as the discrete nature of the propagation constants
given by Eq. (3). Coupling in and out shall be considered
using the general approach discussed in the previous sec-
tion. Thus, we transfer to normalized internal amplitudes
bi (z) and obtain [31]
d α1 ν1
b1 = − b1 − i γ b3 b2∗ e−i mz/R
dz 2 ν3
d α2 ν2
b2 = − b2 − i γ b3 b1∗ e−i mz/R
dz 2 ν3
d α3
b3 = − b3 − iγ b1 b2 ei mz/R
(7)
dz 2
with m = m 3 − m 2 − m 1 . The nonlinear-optical cou-
pling parameter is given by

2 σ123
γ = 2π ν3 d √ (8)
ε0 c03 n 1 n 2 n 3 σ1 σ2 σ3
comprising the respective mode cross sections σi =
i2 dxdy and the overlap cross section σ123 =
1 2 3 dxdy. For simplicity, we use i = m i , pi ,qi .
In the following, we will discuss the phase mismatch
m and the coupling parameter γ in more detail. The ba-
sic structure of the sets (6) and (7) coincide. Thus, also
the solutions will be similar. Solving set (6) yields a nor-
malized conversion efficiency given by sinc2 ( k L/2) [30].
This function is sketched in Fig. 5. It has a global maxi-
mum at k L = 0 and several side maxima with zeros for
even values of k L/π in between. In set (7), k is just
replaced by m/R, thus k L = 2π m. Since m is an
integer, we can expect considerable frequency conversion
for m = 0 only (see Fig. 5). The well-known sinc2 shape

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Figure 5 Normalized efficiency versus phase mismatch k L as
known from the solutions of set (6). The dashed lines indicate the
possible values for m
as known from phase matching nonlinear-optical processes
in bulk crystals doesn’t play a role for three-wave mixing
in whispering gallery resonators.
The condition m = 0 can be satisfied by type-I-
phasematching as demonstrated in Ref. [32]. This requires
unequal polarization directions for the interacting waves
combined with a proper birefringence of the nonlinear-
optical material. A more versatile technique is quasi-
phasematching [33]. It does not restrict the polarization
directions nor birefringence is necessary. However, it re-
quires an additional fabrication step. The crystal structure
has to be modified in such a way that the nonlinear-optical
coefficient varies along the rim as d(z) = d0 S(z). Here, d0
denotes the maximum value of d. The unitless function S(z)
alternates between ±1. It comprises the spatial dependence
of d and since it is periodic in L, it can be represented by a
Fourier series:
+∞
d(z) = d0 S(z) = d0 S M eiM z/R (9)
M=−∞
with the integer M and the corresponding Fourier coeffi-
cients S M . Substituting the constant nonlinear coefficient d
from Eq. (8) by this expression conserves the structure of
the set (7). The nonlinear coefficient d is just replaced by
the effective value |S M |d0 and m = m 3 − m 2 − m 1 − M.
Thus, with a proper choice of S(z) one can ensure m = 0
regardless of polarization directions or birefringence. For
the determination of S M one can use the explicit expression
[34]
N −1
i
SM = (−1) j eiM z j /R (10)
πM j=0
with the respective positions z j of the N domain walls.
Here, the position z 0 is set to zero.
During one roundtrip the polarization direction of the
interacting light fields with respect to the crystallographic
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Figure 6 Function S(z) and corresponding absolute values |SM |
of the Fourier coefficients for different phase matching schemes:
type-I-phase matching (a), quasi-phase matching (b), and 4-
quasi-phase matching (c).
axes might vary. Consequently, an oscillating nonlinear-
optical coefficient can be found in whispering gallery res-
onators without an artificially imprinted quasi-phase match-
ing structure. For example, WGRs made of materials with
4 symmetry provide such a variation in d [35, 36]. These
include the crystal classes 43m (GaAs, GaP, etc.) and 42m
(KD2 PO4 , AgGaSe2 , etc.). Here, we find two Fourier com-
ponents with |S M | = 0.5 at M = ±2. Figure 6 exemplifies
S(z) and the corresponding |S M | for the phase-matching
strategies described above. Summarizing all, we find the
first general selection rule
m3 = m1 + m2 + M (11)
with M = 0 for type-I-phase matching, M = ±2 for 4-
quasi-phase matching and arbitrary integers for quasi-phase
matching.
The parameter γ in set (7) indicates the nonlinear-
optical coupling between the interacting waves. There is
no frequency conversion at all if γ = 0, i.e., for a zero
nonlinear-optical coefficient d or for a zero overlap cross
section σ123 = 1 2 3 dxdy. As mentioned above, the
electric-field distribution  is antisymmetric with respect
to the equatorial plane for odd values of the polar mode
number p and symmetric for even ones. Thus, the product
1 2 3 is antisymmetric if one field or all fields have an
odd polar number. In these two cases the integration over
the cross section gives zero for σ123 . From this symmetry
consideration, we can conclude that the sum p1 + p2 + p3
of the polar mode numbers has to be an even number
in order to ensure a nonzero overlap cross section. Nu-
merically calculating σ123 using Eq. (1) with R = 1 mm,
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Figure 7 Overlap cross section σ123 for R = 1 mm, ρ = 0.25 mm,
m1,2 = 10000, m3 = 20000, q1,2,3 = 1, p1,2 = 0 . . . 10, p3 = 0, 6.
Nonzero values are obtained for p1 + p2 + p3 = 2N and p1 + p2 ≥
p3 only.
ρ = 0.25 mm, m 1 = m 2 = 10000, m 3 = 20000, q1,2,3 = 1,
p1,2 = 0 . . . 10, and p3 = 0 shows this behavior as illus-
trated in Fig. 7. Calculating the overlap cross section for
p3 > 0 reveals another selection rule. The sum p1 + p2
has to be equal or larger than p3 (see Fig. 7). Thus, we can
summarize
p1 + p2 + p3 = 2N , (12)
p1 + p2 ≥ p3 . (13)
We have derived selection rules for m i (Eq. (11)) and
for pi (Eqs. (12, 13)) separately. In a quantum mechanical
approach as used in Ref. [37], the nonlinear-optical cou-
pling strength is proportional to d 1 2 3 dV . Here, the
integration over the volume V reveals all selection rules si-
multaneously. For spherical whispering gallery resonators
and M = 0, they have been derived in Ref. [38] pointing
out that Eqs. (11) and (13) can be interpreted as a conserva-
tion of angular momentum and Eq. (12) as a conservation
of parity.
For spherical WGRs one can abstain from numerical
integration. As demonstrated in Ref. [32], in this situation
it is possible to apply Gaunt’s formula [39] and Stirling’s
approximation for the evaluation of large factorials in order
to obtain the selection rules mentioned above for M = 0.
2.3.2. Input-output relations for three-wave mixing
processes
In the previous section, we have discussed the interaction
between the waves inside the resonator. In order to cal-
culate the output powers as a function of input powers,
we need to supplement the set (7) with relations (4) link-
ing the external amplitudes ai with the internal ones bi
and with proper boundary conditions. This procedure was
successfully applied for second harmonic generation and
optical parametric oscillation in Ref. [31]. It can easily be
adapted to sum and difference frequency generation in order
to obtain input-output relations for all three-wave mixing

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6 I. Breunig: Three-wave mixing in whispering gallery resonators

Figure 8 Efficiency ηsh given by Eq. (17) normalized to its max- Figure 9 Normalized efficiency of sum frequency conversion as
imum value ηsh
max
as a function of pump power Pp normalized to a function of the normalized pump power for different values of B.
max
Pp .

The function X/(1 + X )2 has a maximum value of 0.25 at

X = 1. Thus, we have a maximum achievable efficiency
processes. We will assume that the selection rules (11-13)
are fulfilled. In a first step, all waves are considered to rsh rp
have frequencies perfectly matching whispering gallery res- ηsh
max
= (18)
1 + rsh 1 + rp
onances given by Eq. (2). The influence of detuning from
triple resonance will be discussed subsequently. at the pump power
Second harmonic generation 1 + rp
For frequency doubling, we have only one pump wave with Ppmax = 4 P0 . (19)
rp
the power Pp at the frequency νp . The wave generated has
the power Psh at the frequency νsh = 2νp (see Figure 8). Figure 8 shows this behavior. For realistic parameters
The coupler is described by the respective transmission and νp = 300 THz, n p,sh = 2, d = 1 pm/V, Q 0p,0sh = 5 × 107 ,
coupling coefficients tp,sh and κp,sh . For the output power of
Vp2 Vsh /Vppsh
2
= 106 µm3 and rp,sh = 1, we obtain ηsh max
=
the second harmonic wave, we find [31]
25 % conversion efficiency at Pp = 35 µW pump power.
max

rsh Expressions (15) do not have to be evaluated numeri-

Psh = 4 P0 X 2 with (14) cally. There is a lenghty analytical solution which was used
1 + rsh in Ref. [7] in order to determine an explicit equation for
the conversion efficiency. It is valid for strong overcou-
rp Pp pling where rp,sh 1 and consequently ηsh max
= 1. Com-
X (1 + X )2 = A where A = . (15) bined with a correction indicated in Ref. [32] it perfectly
1 + rp P0 coincides with expression (17).

Expression (15) combines the normalized intracavity Sum frequency generation

power X of the pump wave with the normalized exter- For sum frequency generation (SFG), we have two pump
nal pump power A. The coupling ratios are given by waves with the powers P1,2 at the respective frequencies
rp,sh = κp,sh
2
/αp,sh L with the respective absorption coeffi- ν1,2 . The wave generated has the power Psf at the frequency
cients αp,sh and the power νsf = ν1 + ν2 (see Figure 9). Coupling is described now
by three coefficients κ1,2,sf . Following the notation of Ref.
π ε0 n 4p n 2sh Vp2 Vsh [31], we find for the power of the generated wave
1
P0 = νp (1 + rp )2 (1 + rsh ) .
8d 2 Q 20p Q 0sh Vppsh
2
νsf2 rsf
Psf = 4 P0 X Y with (20)
(16) ν1 ν2 1 + rsf

ν2 r1 P1
Here, n p,sh are the refractive indices of the cavity material X (1 + Y )2 = A where A = , (21)
for the two waves, Q 0p,0sh their intrinsic quality factors, νsf 1 + r1 P0
Vp,sh = σp,sh L their mode volumes, and Vppsh = σppsh L the
ν1 r2 P2
mode overlap volume. Equations (15) can be evaluated nu- Y (1 + X )2 = B where B = . (22)
merically for every pump power Pp in order to get X , which νsf 1 + r2 P0
is then substituted into (14). For the conversion efficiency,
we find As above, the normalized intracavity powers of the pump
waves are given by X and Y whereas A and B denote
Psh rsh rp X the respective normalized external pump powers. The cou-
ηsh ≡ =4 . (17) pling ratios are r1,2,sf = κ1,2,sf 2 /α1,2,sf L with the absorption
Pp 1 + rsh 1 + rp (1 + X )2
coefficients α1,2,sf . The characteristic power P0 is given


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Laser Photonics Rev. (2016) 7

by

ν1 ν2 π ε0 n 21 n 22 n 2sf 1 V1 V2 Vsf
P0 = × ···
νsf 16d 2 2
Q 01 Q 02 Q 0sf V12sf
× (1 + r1 )(1 + r2 )(1 + rsf ) . (23)

Here, the refractive indices n i , the intrinsic quality factors

Q 0i , and the mode volumes Vi are used with the indices
i = 1, 2, sf for the respective waves, while V12sf is the mode
overlap volume. Importantly, for two equal pump beams Figure 10 Normalized conversion efficiencies of optical para-
ν1 = ν2 = νp = νsf /2 and P1 = P2 = Pp /2, the set (20-22) metric oscillation versus the normalized pump power.
transforms exactly to the set (14,15), i.e. to that for second
harmonic generation. by Vpsi . For the conversion efficiencies of this process we
SFG is commonly used for upconverting light at a low find
frequency (let it be ν2 ) to light at a higher frequency νsf
√
in a spectral region where efficient detectors are available. Ps,i νs,i rs,i rp N −1
Thus, it makes sense to define the conversion efficiency as ηs,i ≡ =4 (28)
Pp νp 1 + rs,i 1 + rp N

Psf νsf rsf r2 X with N = Pp /Pth representing the pump power √ normal-
ηsf ≡ =4 (24) ized to the oscillation threshold. The function ( N − 1)/N
P2 ν2 1 + rsf 1 + r2 (1 + X )2
in the conversion efficiency is a general feature of multi-
As for second harmonic generation, the efficiency for resonant optical parametric oscillators [3]. It has a maxi-
SFG has a maximum value mum value of 0.25 at N = 4. Thus the conversion efficiency
reaches the maximum value
νsf rsf r2
ηsfmax = (25) νs,i rs,i rp
ν2 1 + rsf 1 + r2 ηs,i
max
= (29)
νp 1 + rs,i 1 + rp
at the pump power
at the pump power
 2
νsf 1 + r1 B
P1max = P0 1 + . (26) Ppmax = 4Pth . (30)
ν2 r1 4
This behavior is illustrated in Fig. 10. For strong over-
This behavior was described in Ref. [40], just using a differ- coupling (r j 1) the last factor comprising the coupling
ent notation. Figure 9 shows the conversion efficiency ηsf ratios in expression (27) can be set to unity when the in-
as a function of the pump power P1 . Importantly, at input trinsic quality factors Q 0 j are replaced by the loaded ones.
powers P2 leading to B > 4 a bistable behavior is found The resulting compact equation for the oscillation threshold
around P1max with the maximum efficiency located on an was determined in Ref. [42]. The general influence of the
unstable branch. This is known also for doubly resonant coupling ratio on the pump threshold and on the conversion
sum frequency generation [41]. efficiency described by Eqs. (27) and (28) perfectly coin-
cides with the one that was determined for triply resonant
Optical parametric oscillation optical parametric oscillators based on mirror cavities [43].
An optical parametric oscillator (OPO) is pumped with
the power Pp at the frequency νp . The OPO generates two Difference frequency generation
waves (signal and idler) with the respective powers Ps,i In order to complete the picture, we consider the fourth
at frequencies νs,i when the pump power overcomes the three-wave mixing process, i.e. difference frequency gen-
oscillation threshold [31] eration, also employing the notation of Ref. [31]. Here, we
have two input waves (pump and signal) with the powers
π νp ε0 n 2p n 2s n 2i 1 Vp Vs Vi Pp,s at the frequencies νp,s . The third wave (idler) is gen-
Pth = × ···
16d 2 2
Q 0p Q 0s Q 0i Vpsi erated with the power Pi at νi = νp − νs . This process can
be considered as seeded optical parametric oscillation. The
(1 + rp )2 (1 + rs )(1 + ri ) power of the idler wave is given by
× (27)
rp
νi ri
Pi = 4 P0 X Y with (31)
where the refractive indices n i , the intrinsic quality fac- νs 1 + ri
tors Q 0i , the mode volumes Vi and the coupling ratios ri
have the indices i = p, s, i denoting the pump, signal, and νs rp Pp
X (1 + Y )2 = A where A = , (32)
idler waves, respectively. The overlap volume is indicated νp 1 + rp P0

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8 I. Breunig: Three-wave mixing in whispering gallery resonators

Figure 11 Normalized conversion efficiency of difference fre-

quency generation versus normalized pump power for different
Figure 12 The frequencies νp,s,i are close to resonances at νmp,s,i
values of B.
with the widths νp,s,i and the normalized detunings δ̂, δ̂p . The
circles denote signal and idler frequencies that would fulfill fre-
quency and phase matching condition. Only at the frequencies
rs Ps
Y (1 − X )2 = B where B = . (33) indicated by the filled circles the normalized detunings of signal
1 + rs P0 and idler are equal.

As before, Eqs. (32) and (33) combine the normalized For the characteristic powers maximizing the conversion
intracavity powers X and Y with the respective external efficiency, we compare Eqs. (19), (26), (30), and (37). Also
values A and B. The characteristic power is given by here, we have a similar behavior for all processes:
π ε0 n 2p n 2s n 2i 1 Vp Vs Vi
P0 = νs × ··· (1 + r )4
16d 2 2
Q 0p Q 0s Q 0i Vpsi P max ∝ . (39)
r
× (1 + rp )(1 + rs )(1 + ri ). (34) From these two expressions, we can conclude that high
efficiencies are reached at strong overcoupling whereas the
Because of the close relation to optical parametric oscilla-
lowest characteristic pump powers are found in the regime
tion, we define the conversion efficiency as
of slight undercoupling.
Pi νi rp ri Y
ηi ≡ =4 . (35) Influence of detuning
Pp νp 1 + rp 1 + ri (1 + Y )2
So far, we have assumed that all interacting waves are per-
Thus, the conversion efficiency of difference frequency gen- fectly resonant. The influence of detuning on the conversion
eration reaches a maximum value efficiency and on the characteristic pump power was dis-
cussed in Refs. [34] and [44] for optical parametric oscilla-
νi rp ri tion in whispering gallery resonators. Let us assume that the
ηimax = (36)
νp 1 + rp 1 + ri frequencies νp,s,i are detuned by δνp,s,i from the resonance
frequencies νm p,s,i with the respective widths νp,s,i such
at the power that the phase matching condition m p = m s + m i + M is
  perfectly fulfilled (see Fig. 12). In the following, we will use
νp 1 + rp the normalized detunings δ̂p,s,i = 2δνp,s,i / νp,s,i indicating
Ppmax = 4 P0 1 − B . (37)
νs rp how many half linewidths the frequencies are detuned from
the respective resonances.
Figure 11 shows this behavior. Importantly, for B = 0, Signal and idler frequencies have to be perfectly cen-
we obtain exactly the result of optical parametric oscillation tered around the point of degeneracy at νp /2 in order to
with the pump threshold at Ppmax /4. fulfill the frequency condition νp = νs + νi . Due to disper-
sion, this is not necessarily true for the resonance frequen-
Influence of coupling cies νm p,s,i . From figure 12 it becomes clear that one finds
All three-wave mixing processes reach a maximum conver- an infinite number of possible frequency combinations νs,i
sion efficiency at a certain characteristic pump power. The around their resonances that all fulfill the frequency condi-
values of both strongly depend on the coupling ratios r j tion. However, the parametric oscillation will occur only at
of the interacting waves. Although the coupling ratios are the one combination that ensures
generally unequal, it is very instructive to consider them as
equal r j = r . Comparing Eqs. (18), (25), (29), and (36), we δ̂s = δ̂i ≡ δ̂ . (40)
see that the maximum conversion efficiency of three-wave
mixing processes is Thus, this expression can be interpreted as a single-
frequency condition. It is a general feature of all nonde-
r2 generate doubly and triply resonant optical parametric os-
ηmax ∝ . (38)
(1 + r )2 cillators [45, 46]. Importantly, the normalized detunings of


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Laser Photonics Rev. (2016)
pump and generated waves cannot be treated as indepen-
dent parameters. They are connected via δ̂p = (δ̂ − δ̂0 )
with = ( νs + νi )/ νp . Here, δ̂0 is the normalized
detuning of the generated waves for a perfectly resonant
pump wave.
Nonzero detunings from the resonances increase the
oscillation threshold as
 
Pthδ = Pth 1 + δ̂p2 (1 + δ̂ 2 ). (41)
Considering that Pth can be of the order of microwatts
in typical whispering gallery resonators, we can expect to
drive optical parametric oscillation even when all waves
are detuned by several half linewidths from their respective
resonance frequencies. Of course, the maximum efficiency
will drop in this case.
There is another important issue implied by detuning.
The pump power transmission as a function of pump de-
tuning strongly deviates from a lorentzian shape when the
oscillation threshold is overcome. This is due to the fact that
the three-wave mixing process acts as an additional loss for
the pump wave. Thus, it affects the coupling efficiency
and hence the transmission signal. This effect is discussed
for triply resonant optical parametric oscillators with mir-
ror resonators [46] and with whispering gallery resonators
[44]. It is necessary to take it into account when stabilizing
actively the resonator in order to achieve continuous-wave
output emission.
3. Resonator fabrication
3.1. Generating quasi-phase-matching
structures
As discussed in section 2.3.1, quasi-phase matching en-
ables the fulfillment of the selection rule (11) for every
combination of polarizations or frequencies. The price of
Figure 13 (a) Sketch of a radial domain structure for quasi-phase matching in a WGR. The red circle indicates the propagation path
of the light and ± the sign of the nonlinear-optical coefficient. (b) Crystallographic axes in the xy plane for lithium niobate crystals.
(c) Radial domain structures in lithium niobate without and (d) with optimization of the poling process. The patterns are visualized by
etching with hydrofluoric acid. The domain walls appear dark blue.
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9
this flexibility is the necessity of an additional fabrication
step. The material has to be structured in such a way that
the nonlinear-optical coefficient varies along the rim. Ba-
sically, the techniques known from conventional devices
where the light propagates along a straight line [47] can be
applied to whispering gallery resonators as well: electric-
field poling for ferroelectric crystals like lithium niobate
and orientation-patterned growth for semiconductors like
gallium arsenide. So far, all experiments on quasi-phase-
matched three-wave mixing in WGRs are conducted with
ferroelectrics.
Due to the circular path of the light, a radial quasi-
phase-matching structure as sketched in Figure 13a most
naturally mimics the parallel stripes known from conven-
tional devices. Here, the domains are aligned in different di-
rections with respect to the crystallographic axes (Fig. 13b).
In lithium niobate crystals, the domain growth is strongly
anisotropic. Experimentally realized radial patterns show
domains aligned along the y-axis that are much thinner
than the ones aligned along the x-axis [48] (Fig. 13c). Cal-
ligraphic poling [49], i.e. domain switching by moving a
charged metal tip across the crystal, provides an elegant so-
lution. Here, poling conditions like voltage or speed of the
tip can be easily adopted to the writing direction. Such an
optimization leads to radial patterns with almost uniform
domains [50] (Fig. 13d).
Furthermore, it was demonstrated that the humidity of
the environment of the tip significantly influences the do-
main switching process [51]. Radial domain patterns in
lithium niobate crystals have been realized also by uv-light
assisted poling [48, 52].
Quasi-phase matching structures with parallel domains
are much easier to fabricate and commercially available.
They comprise a broader Fourier spectrum than the ra-
dial ones [53]. Thus, they can be used for broadband
quasi-phase matching. However, one has to take into ac-
count the reduced effective nonlinear-optical coefficient.

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10 I. Breunig: Three-wave mixing in whispering gallery resonators

In order to obtain a compromise between simple fabrica-
tion and high nonlinearity, patterns comprising six regions
with parallel domains aligned along the y-axes have been
proposed [54].
3.2. Resonator shaping
3.2.1. Bulk resonators
For the first demonstration of three-wave mixing in a whis-
pering gallery resonator, the spheroidal cavity was made of
a bulk lithium niobate crystal [7]. The latter is transformed
into a WGR in several steps. First, a cylindrical preform
is drilled out of the material. Then, the rim of the preform
is shaped on a lathe or by hand. Finally, the rim around
the equator is polished by hand using adequate slurries.
This procedure was adopted to various other second-order
nonlinear optical materials, such as quartz [55], lithium tan-
talate [56], beta-barium borate [57], and lithium tetraborate
[58]. For all materials, the quality factor of the resonator
is of the order of 108 to 109 and limited by material ab-
sorption. Mechanical polishing ensures a residual surface
roughness in the nm range or below. This procedure is ap-
plied for the fabrication of whispering gallery resonators
with radii down to several 10 µm [59].
If a WGR is fabricated out of a chip with a radial QPM
structure, one has to keep in mind that the center of the
resonator should coincide with the one of the radial pattern.
Otherwise, the periodicity will vary along the rim. This
will reduce the effective nonlinear optical coefficient and
broaden the Fourier spectrum of the pattern. For millimeter-
sized resonators, a displacement of tens of µm already has
a substantial impact [54, 60].
3.2.2. On-chip resonators
For the fabrication of small whispering gallery resonators
that allow their integration on chips, lithographic fabri-
cation techniques are applied. In lithium niobate crystals,
ring resonators have been fabricated via proton exchange
[61] and titanium diffusion [62]. These devices measured
2.5 mm and 80 mm in diameter, respectively, providing
quality factors of 105 and 106 . In both examples, the rings
were not etched. The light was guided in the region of
increased refractive index only.
In order to reduce the resonator size, the refractive-index
difference between the guiding structure and its vicinity
has to be larger than the one provided via proton exchange
and titanium diffusion alone. Thus, etching is necessary.
Combining refractive-index enhancement with subsequent
etching, ring resonators with 200 µm diameter and a quality
factor of about 104 have been demonstrated [63, 64].
Thin films of lithium niobate on a substrate [65] (also re-
ferred to as lithium-niobate-on-insulator) provide a prefer-
able platform for the fabrication of integrated whispering
gallery resonators. By etching rings or disks into the lithium
niobate films, WGRs with diameters of several 10 µm with
quality factors up to 106 were realized [66–71].
For other second-order nonlinear optical materials such
as (aluminum)gallium arsenide, gallium phosphide, and
gallium nitride a similar approach is applied. Thin films
of these materials are bonded on a substrate or deposited by
molecular beam epitaxy. Subsequently, rings or disks are
etched into the films. Using this technique, ring resonators
made of gallium arsenide [72] and gallium nitride [73,74] as
well as disk resonators made of aluminum gallium arsenide
[75, 76], gallium arsenide [75, 77] and gallium phosphide
[78] have been fabricated. These devices typically measure
between several and several tens of micrometers in diameter
providing quality factors between 104 and 106 .
Compared with their bulk counterparts, the chip-
integrated WGRs demonstrated so far have two orders of
magnitude lower quality factors. This is due to the resid-
ual surface roughness after the etching process. Figure 14
shows a collection of whispering gallery resonators with
different shapes made of various materials.

Figure 14 Whispering gallery resonators fabricated out of various non-centrosymmetric materials. Picture a) is reprinted with kind
permission from [7]. Copyright 2004 by the American Physical Society. Pictures b, f, h, j) are reprinted with kind permission of the
Optical Society of America from [57, 58, 68, 76]. Pictures c, d) are reprinted with kind permission from [67, 72]. Copyright 2010, 2000
by IEEE. Pictures e,i) are reproduced from [74, 75] with the kind permission of AIP Publishing. Picture g) was kindly provided by C.
Marquardt from the Max Planck Institute for the Science of Light, Erlangen, Germany.


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Laser Photonics Rev. (2016) 11

structure varies along the rim. However, it ensures phase

Figure 15 Sketch of the first demonstration of SHG in a WGR
made of bulk periodically-poled lithium niobate (left). While scan-
ning the pump frequency, the transmitted pump light at 1550 nm
wavelength as well as the generated second harmonic light at
775 nm wavelength are detected (right). The data were taken
from Ref. [7].
4. Experiments on three-wave mixing
4.1. Frequency doubling
Frequency doubling in a whispering gallery resonator was
demonstrated in 2004 for the first time [7]. In this experi-
ment, pump light at 1550 nm wavelength was converted to
light at 775 nm wavelength with up to 50% efficiency at
25 mW pump power only. The millimeter-sized resonator
was made of a periodically-poled lithium niobate crystal
(see Fig. 15). Thus, phase matching was not optimized for
this particular process, since the periodicity of the QPM
matching over a broad wavelength range. This was con-
firmed by frequency doubling of 1319-nm-wavelength light
in the same resonator.
The frequency-doubling experiments published so far
base on a similar setup and on the same procedure: The fre-
quency of the pump light is scanned across the resonances
of the cavity and simultaneously the transmitted pump light
as well as the generated second harmonic light are detected.
Literature data are compared in Table 1 in terms of
resonator material, resonator radius R, wavelength λsh of
the generated light, slope efficiency ηs , maximum efficiency
ηmax reached, and phase-matching strategy.
Whispering-gallery based frequency doublers success-
fully generate light from the ultraviolet (245 nm wave-
length) to the infrared (942.5 nm wavelength).
In terms of efficiency, there is a huge difference be-
tween bulk and on-chip devices (examplified in Fig. 16).
Bulk WGRs enable conversion efficiencies typically rang-
ing from several to several ten percent at milliwatt powers
even with non-optimized but broadband phase matching
in beta barium borate (BBO) [79] or with lithium tetrabo-
rate (LB4) having a nonlinear-optical coefficient as tiny as
0.073 pm/V [58]. 9% conversion efficiency at only 30 µW
pump power has been demonstrated with optimized bire-
fringent phase matching in a WGR made of bulk lithium
niobate [32]. These results highlight the potential for WGRs
as miniaturized efficient frequency converters.
In contrast to this, the slope efficiencies as well as the
maximum efficiencies of on-chip devices are two to three

Table 1 Experimental demonstrations of frequency doubling in WGRs comparing the respective non-centrosymmetric materials, radii
R, second-harmonic wavelengths λsh , slope efficiencies ηs , maximum efficiencies ηmax at pump powers Pp , and phase matching
schemes. Bulk and on-chip resonators are indicated by (b) and (oc), respectively, and non-optimized but broadband phase matching
by ∗ . The phrase q modes“ expresses phase matching via different mode numbers q for pump and second harmonic waves. As a
reference, experimental results of frequency doubling in waveguides (wg) are included. Here, the waveguide length indicated followed
by ∗∗ .

Material R [µm] λsh [nm] ηs [%/mW] ηmax [%] @ Pp [mW] Phasematching Ref.
LN (b) 1500 775 50 @ 25 QPM∗ [7]
659.5 2 @ 30
LN (b) 1900 532 9 @ 0.03 BPM [32]
∗
BBO (b) 910 778.5 0.063 0.069 @ 1.1 BPM [79]
487 4.6 1.15 @ 0.25
435 1.8 1.57 @ 0.87
317 0.74 0.31 @ 0.42
LB4 (b) 1150 245 0.37 2.2 @ 6 BPM
LN (oc) 14 773 2 × 10−4 3.8 × 10−4 @ 1.8 unclear [68]
LN (oc) 41 400 1.3 × 10−3 8 × 10−3 @ 6 unclear [71]
GaAs (oc) 2.6 942.5 5 × 10−3 4 × 10−4 @ 0.08 4QPM [77]
AlGaAs (oc) 2 792 7 × 10−5 1.4 × 10−4 @ 2 4QPM [80]
GaN (oc) 80 780 2 × 10−5 2 × 10−3 @ 100 q modes [73]
LN (wg) 60000∗∗ 775 1.4 45 @ 900 QPM [81]
LN (wg) 50000∗∗ 780 2.4 92 @ 160 QPM [82]

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Figure 16 Conversion efficiency versus pump power for fre-
quency doubling laser light around 1550 nm wavelength in a bulk
WGR and in an on-chip WGR. The data were taken from Ref. [7]
and [73].
orders of magnitude lower. Looking at Eq. (17) in the un-
depleted pump approximation (X  1), we see that the
slope efficiency ηs ≡ ηsh /Pp isproportional to Q 3 /V with
V being the effective mode volume. The quality factors
and mode volumes are roughly two orders of magnitude
smaller than the ones of bulk resonators. The other pa-
rameters can be similar. Thus, the limited quality factor of
on-chip WGRs explains the four orders of magnitude lower
conversion efficiencies compared with that of bulk devices.
It makes sense to compare the conversion efficiencies of
WGR based devices with that of waveguides which can also
be integrated on a chip. The latter are typically several cm
long and provide ηs = (1 . . . 2) %/mW [81,82]. Their max-
imum conversion efficiency can exceed 90% [82]. These
values outnumber the ones of the state-of-the-art on-chip
WGRs by far. However, looking at the respective values
for bulk WGRs and especially at the ones presented in
Ref. [32], the advantage of WGR based devices in terms of
slope efficiency becomes obvious. One can estimate from
ηmax = 9% reached at 30 µW pump power that ηs is of the
order of several 100%/mW which is two orders of magni-
Figure 17 (a) Spectrum of the first proved WGR-based OPO. (b) Power Ps + Pi versus the pump power of the same experiment (b).
The solid line represents a fit of Eq. 28 to the experimental data indicating an oscillation threshold Pth = 6.7 µW, which is still the
lowest pump threshold of an OPO observed so far. Data were taken from Ref. [86].

C 2016 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
I. Breunig: Three-wave mixing in whispering gallery resonators
tude larger than the values obtained with waveguides. The
reason for this is the following: Both concepts, WGRs and
waveguides provide roughly the same mode cross section,
however WGRs add a substantial power enhancement due
to resonance. This can be achieved in waveguides also with
additional high-reflective coatings.
Remarkably, frequency doubling was observed in a
on-chip WGR made of silicon nitride (SiN) which is a
centrosymmetric material. The ring in this experiment
measured 116 µm in diameter. Light at 777.1 nm wave-
length was generated with ηs = 10−4 %/mW and ηmax =
3.2 × 10−3 % at 320 mW pump power [83]. These values
are of the same order as the other ones obtained with on-chip
resonators made of non-centrosymmetric materials. The
second-order nonlinearity in this experiment is attributed
to a break of symmetry at the surface of the resonator [84].
Also covering the surface of a whispering gallery res-
onator made of glass (360 µm diameter) with a monolayer
of crystal violet molecules enables frequency doubling [85].
In this experiment, violet light at 400 nm wavelength was
generated. The molecules were deposited with a periodical
pattern around the equator in order to mimic a quasi-phase-
matching structure as known from non-centrosymmetric
crystals.
4.2. Optical parametric oscillation
First indications of highly nondegenerate optical parametric
oscillation generating idler light with frequencies of several
hundred Gigahertz in a whispering gallery resonator have
been published in 2007 [87]. In this experiment, the cavity
measuring 840 µm in diameter was made of bulk lithium
niobate. However, the idler light could not be detected di-
rectly. The first proof of optical parametric oscillation in a
WGR was published three years later [86]. Here, the three-
wave mixing process was pumped at 532 nm wavelength
generating signal and idler waves at 1012 and 1123 nm
wavelengths, respectively (see Fig. 17).
In contrast to frequency doubling, all WGR OPOs
demonstrated so far are based on millimeter-sized cavities
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Figure 18 Whispering gallery optical parametric oscillator
pumped at 450 nm wavelength generating orange and infrared
light (a). Wavelength ranges covered by WGR OPOs pumped at
450, 488, 532 and 1040 nm wavelengths, respectively (b).
made of bulk lithium niobate crystals. They are pumped in
the visible at 450, 488, or at 532 nm wavelengths employ-
ing type-I-phasematching [44, 88, 89]. Devices pumped at
1040 nm wavelength require quasi-phase matching [60].
Coarse wavelength tuning over hundreds of nanometers is
achieved via varying the temperature of the resonator or
by varying the pump mode number. Figure 18 summarizes
the tuning range of state-of-the-art WGR OPOs. The wave-
lengths of the light generated ranges from 571 nm (pumped
in the blue) to 2600 nm (pumped in the infrared). Using
temperature tuning only, WGR OPOs can be applied for
broadband spectroscopy [50].
There are several strategies for fine (mode-hop free)
tuning the wavelengths of the generated light [90]: apply-
ing an external electric field, applying mechanical stress, or
manipulating the evanescent fields of the circulating waves.
Combining these strategies with the coarse tuning (wave-
length jumps by changing the resonator temperature), it
is possible to tune the output wavelengths in a controlled
way until they meet MHz-wide resonances of alkali atoms
[91]. Thus, wavelength tuning of whispering-gallery-based
OPOs can be controlled at a level that is sufficient for high-
resolution spectroscopy. It is highly remarkable that this is
achieved despite of the intrinsic triple resonance and despite
of the fact that all waves are influenced simultaneously.
As indicated by the theoretical expressions (38) and
(39), the oscillation thresholds and conversion efficien-
cies of WGR-based OPOs strongly depend on the coupling
regime. Just by varying the gap between coupler and res-
onator, the oscillation threshold is changed from 200 µW
(slight undercoupling) to 4 mW (strong undercoupling),
whereas the conversion efficiency ranges between 10−2 %
(strong undercoupling) and 30 % (overcoupling) [92]. The
lowest oscillation thresholds observed so far are in the low
µW range [86], while the highest conversion efficiency ex-
ceeds 50% [93].
Most experiments on optical parametric oscillation in
WGRs are conducted by scanning the pump frequency forth
and back across a pump resonance, i.e., the same procedure
as used for frequency doubling. Consequently, the output
comprises millisecond long light flashes instead of continu-
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13
ous radiation. The latter was achieved by locking the pump
laser to a resonance and controlling the resonator temper-
ature on a mK level [93]. For the locking one has to take
into account the deformation of the pump mode due to the
parametric process [44].
Besides for classical spectroscopy as mentioned above,
WGR based OPOs are suitable sources for nonclassical
light [94]. Below the oscillation threshold, i.e. in the re-
gion of spontaneous parametric down conversion, they are
applied as a source for single photon pairs as well [95, 96].
4.3. Other processes
Besides frequency doubling and optical parametric oscil-
lation also sum frequency generation as well as cascaded
three-wave mixing processes have been demonstrated in
millimeter-sized bulk whispering gallery resonators made
of lithium niobate crystals. As mentioned in section 2.3.2
SFG can be applied for upconverting light from the infrared
to the visible spectral region where the most efficient de-
tectors are available. The WGR-based system presented in
Ref. [40] was pumped at 780 nm wavelength converting
signal light at 1560 nm to radiation at 520 nm wavelength
via SFG. The efficiency P520 /P1560 exceeded 2.5 × 10−3 at
a pump power P780 below 1 mW.
This scheme could be very useful for the detection of
far-infrared (THz) radiation as discussed in [97]. The first
step into this direction was demonstrated in Ref. [98]. Here,
0.4 mW of cw radiation at 100 GHz frequency were upcon-
verted into the near infrared with 5 × 10−3 power efficiency
corresponding to 2.6 × 10−6 photon number efficiency at
a pump power of 16 mW. It should be noted that this ex-
periment is not SFG in a WGR in a strict sense since the
far-infrared radiation was not coupled into the resonator. It
has modulated the refractive index of the lithium niobate
disk via the electro-optic effect from outside.
Recently, microwaves of 10 GHz frequency have been
upconverted into the optical-telecommunication range by
applying a similar strategy [99]. Here, a photon number
efficiency of 0.1% was achieved by pumping the millimeter-
sized WGR made of lithium niobate with 1 mW power at
1550 nm wavelength. The input power of the microwave
was in the microwatt range only.
Cascaded three-wave mixing processes are useful, e.g.,
for the generation of the third harmonic, where frequency
doubling (ν → 2ν) is followed by sum frequency genera-
tion (ν + 2ν → 3ν). Such a cascade (1554 nm → 777 nm
→ 518 nm wavelengths) was demonstrated in a WGR with
a radial QPM structure not optimized for this particular
process[100]. Nevertheless, conversion efficiencies around
2% for frequency doubling and 0.2% for frequency tripling
were reached.
A longer cascade (1536 nm → 768 nm → 512 nm →
384 nm wavelengths) was realized for the generation of ul-
traviolet light [101]. Here, broadband quasi-phase matching
via a parallel domain structure was applied. The combina-
tion of such a cascade with stimulated Raman scattering can

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Figure 19 Output spectrum between 300 and 900 nm wave-
length of a cascaded three-wave mixing process pumped at
1536 nm wavelength. The main peaks arise from frequency dou-
bling, tripling and quadrupling of the pump wave. The other com-
ponents can be attributed to Raman scattering. The data were
taken from Ref. [102].
be used to generate laser light at more than 20 wavelength
components simultaneously between 375 and 851 nm (see
Fig. 19) in a millimeter-sized WGR at 200 mW pump power
only [102].
4.4. Comparison of experimental results with
theoretical predictions
In the following section, we want to discuss how well the
experimental results fit to the theoretical predictions made
by the input-output relations summarized in section 2.3.
First, we start with the dependence of the conversion effi-
ciency as a function of input power. For all basic three-wave
mixing processes, we expect that the efficiency reaches
a maximum at a certain pump power before it decreases
again. This behavior fits nicely to observations for second
harmonic generation [7] and for optical parametric oscil-
lation [86, 88]. In some experiments only a saturation of
the conversion efficiency was observed [32, 40]. A reason
might be that at high pump powers, additional processes
or multi-mode operation occur. Since the theoretical model
described above is only valid for a single three-wave mixing
process it might fail to describe the experimental results at
high pump powers.
Now, we want to switch to the influence of the coupling
ratio ri on the conversion efficiency and on the characteristic
pump power maximizing the conversion efficiency. So far,
there is only one systematic study about this for optical
parametric oscillation [92]. It shows that the conversion
efficiency grows monotonically with increasing coupling
strength, whereas the smallest pump threshold is found
at slight undercoupling. The experimental results are well
described by Eqs. (27) and (28).
Furthermore, the influence of detuning on the oscilla-
tion threshold of an optical parametric oscillator given by
Eq. (41) and the corresponding deviation of the line shape

C 2016 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
I. Breunig: Three-wave mixing in whispering gallery resonators
of the pump light from a lorentzian fits perfectly to experi-
mental observations [20].
Thus, all theoretical predictions for basic influences of
pump power, of coupling strength and of detuning on the
conversion efficiency as well as on the oscillation thresh-
old of optical parametric oscillators have been verified
experimentally. However, the quantitative comparison of
the oscillation threshold itself is still an issue. A closer
look at Eq. (27) gives the explanation. For the calculation
of the oscillation threshold, we need to know the effec-
tive mode volume and consequently, the mode numbers p
and q of all three waves. For the pump wave, the num-
bers can be determined by a spectral fit of Eq. (2) to the
pump spectrum [24]. However, so far there is no exper-
imental demonstration of the unambiguous determination
of the mode numbers for the two generated waves. Thus,
a quantitative comparison of the theoretically predicted
oscillation threshold with the experimental values is still
missing.
5. Material considerations
In order to compare non-centrosymmetric materials re-
garding their applicability for three-wave mixing, a fig-
ure of merit is defined as F O M = d 2 /n 3 [103]. This def-
inition is useful if absorption of the material can be ne-
glected. For conventional devices with a mirror cavity or
without a cavity at all, this is valid over the entire trans-
parency range of the material. However, in WGR-based
devices, the intrinsic quality factor Q 0 and thus the ab-
sorption plays a major role. From expressions (16), (23),
(27), and (34) it becomes obvious that the characteristic
pump power for any three-wave mixing process is pro-
portional to n 21 n 22 n 23 /(d 2 Q 01 Q 02 Q 03 ). Thus, a proper fig-
ure of merit for a material used in a WGR-based device
would be
d2
FOM = Q 01 Q 02 Q 03 . (42)
n6
In this definition, it is assumed that the refractive index
of the material does not vary much in the transparency
range. However, for the intrinsic quality factor, the wave-
length dependence has to be considered. Figure 20 shows
Q 0 for whispering gallery resonators made of lithium nio-
bate versus the wavelength. In the nominal transparency
range between 0.32 and 5 µm wavelength, Q 0 varies over
several orders of magnitude. Pronounced dips in the qual-
ity factor originate from iron or hydrogen impurities left
from the growth process [104]. Thus the figure of merit
strongly depends on the respective wavelengths of the three
interacting fields.
The figure of merit as defined in (42) highlights an im-
portant circumstance: a tiny nonlinear-optical coefficient
is compensated by a high intrinsic quality factor. Conse-
quently, materials that are only rarely applied in standard
three-wave mixing experiments because of their low value
of d can be very useful for WGR-based systems. This was
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Laser Photonics Rev. (2016)
Figure 20 Quality factor of a whispering gallery resonator made
of lithium niobate for extraordinarily polarized light. The values are
calculated from absorption data [104]. The dips around 2.5 µm
wavelength are attributed to absorption stemming from residual
hydrogen.
confirmed by efficient frequency doubling in a WGR made
of lithium tetraborate having d = 0.073 pm/V only [58].
Absorption does not only determine the characteristic
pump power of a WGR-based three-wave mixing process,
but also its stability. Absorption induces thermal heating
of the WGR and consequently mode drifts and probably
detuning from perfect triple resonance.
The great majority of WGR-based three-wave mixing
experiments is conducted with lithium niobate crystals.
Here, one has to be aware of the photorefractive effect also
called optical damage [105]. Absorption of visible light
leads to generation of mobile charges that are redistributed
creating electric space charge fields and, via the electro-
optic effect, refractive index changes that disturb the circu-
lating light. Mode drifts and mode crossings in WGRs made
of lithium niobate have been attributed to photorefractiv-
ity [106, 107]. Such behavior greatly limits the stability of
WGR-based devices. Unwanted refractive-index changes
in lithium niobate can also be generated via the pyroelec-
tric effect [108]. A solution of this material problem is the
use of periodically-poled lithium niobate crystals. Here,
the photorefractive damage is significantly reduced [109]
compared with that of single domain crystals.
As mentioned above, external electric fields can be ap-
plied in order to fine-tune the resonant frequencies via the
electro-optic effect. Here, one has to take into account that
the material might be photoconductive [110, 111], i.e., the
electric field generating the desired refractive index de-
creases with time while the characteristic decay rate in-
creases with light power. Such a behavior has been observed
in WGRs [90]. It considerably limits the tuning possibil-
ity with a static electric field. Both photorefraction as well
as photoconductivity strongly depend on wavelength. For
lithium niobate, they are much stronger in the visible than
in the infrared range. Thus, in the latter these two effects
will not seriously affect a three-wave mixing process in a
WGR.
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15
6. Conclusion and perspectives
In their first decade of existence, frequency converters based
on three-wave mixing in whispering gallery resonators have
proven to combine efficiencies of up to several tens of
percent at milliwatt input powers with compactness. These
monolithic devices measure from several micrometers to
several millimeters in diameter only. They are successfully
operated from the ultraviolet to the near infrared. As optical
parametric oscillators, they generate single-frequency light
tunable over hundreds of nanometers. Furthermore, they
are applied also for light detection.
The experiments on bulk WGRs have revealed the high-
est efficiencies and, even more important, the possibility to
control the tuning behavior to a level that is sufficient for
broadband as well as for high-resolution spectroscopy in
spite of the intrinsic triple resonance. This demonstration
greatly enhances the probability that frequency converters
based on WGRs will find the way out of labs into commer-
cial applications.
In order to pave the way for this, further progress in
WGR manufacturing is required. So far, the bulk resonators
rely on hand-polishing in the final step while the on-chip
resonators show two orders of magnitude lower intrinsic
quality factors. Completely machine-made WGRs based
on non-centrosymmetric crystals with quality factors ex-
ceeding 108 would be a major achievement. Heating the
materials close to their respective melting points and keep-
ing this temperature for several hours as demonstrated in
[112] might be used as a final fabrication step for resonators
in order to improve the surface roughness.
As mentioned above, the fabrication of WGRs out of
a wafer with a radial quasi-phase-matching structure is not
an easy task. The center of the resonator and the center of
the domain pattern have to match with an accuracy better
than 10 µm. A new strategy could be valuable here. It was
demonstrated that ferroelectric domains in lithium niobate
can be switched directly using a focused ultraviolet laser
beam [113]. This works on the x and on the y face of the
crystal [114]. Using such a technique, one can imprint the
QPM structure directly below the rim after the resonator
was shaped and polished.
So far, QPM was applied in WGRs made of lithium nio-
bate only. Recent progress in the fabrication of orientation-
patterned semiconductors as gallium arsenide [47], gal-
lium phosphide [115], and gallium nitride [116] gives
hope that the wavelength range of frequency convert-
ers based on WGRs will be extended greatly. Especially
gallium arsenide and gallium phosphide enable opera-
tion in the mid and even in the far infrared. The effi-
ciency of cascaded three-wave mixing processes in WGRs
could be boosted by using aperiodic QPM structures
[47, 117] that are optimized for a specific cascade instead
of broadband QPM.
A combination of several strategies can be used to tune
the wavelength of WGR-based OPOs in a controlled way.
However, systematic investigations regarding the tuning be-
havior of these devices via mechanical pressure [118, 119]
or via influencing the evanescent field of the interacting

C 2016 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
 LASER
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REVIEWS
16
Figure 21 A cascade of second harmonic generation (SHG), op-
tical parametric oscillation (OPO) and sum frequency generation
(SFG) generates frequency combs around νp and 2νp . a) SHG
of the pump wave at νp and subsequent OPO generate two fre-
quency components centered around νp . b) The latter are trans-
fered to frequency components centered around 2νp via SFG and
SHG. The sketch is adopted from Ref. [123].
waves [90] are still missing. These two strategies are of
major importance for all devices based on quasi-phase
matching since the domain pattern will hamper the tuning
by applying an external electric field using simple surface
electrodes.
In contrast to their mirror-based counterparts, WGR-
based frequency converters have not been operated with
biaxial crystals yet. The special feature of a WGR made of
a biaxial crystal is the missing rotational symmetry, since
the refractive index might vary along the rim. Consequently,
there will be no conservation of angular momentum and the
phase-matching condition (11) cannot be applied anymore.
We can expect a completely different tuning behavior. So
far, there is no proper theoretical model describing three-
wave mixing in such WGRs.
Besides the application for conventional frequency con-
version (SHG, SFG, OPO, DFG), WGR-based three-wave
mixing devices have been discussed to serve for optical
switches, where pump light and signal light do not directly
interact with each other [120]. Another future application
might be the generation of frequency combs. In the past,
they have been realized in WGRs made of centrosymmet-
ric materials, thus relying on the third-order nonlinearity
[121]. Recently, it was demonstrated that cascading fre-
quency doubling and optical parametric oscillation mimics
a third-order nonlinearity generating a frequency comb as
well [122,123]. This scheme is sketched in Fig. 21 and it can
be transfered to whispering gallery resonators [124, 125].
As for frequency tripling, one can expect that the frequency
comb generation via a cascade of two second-order nonlin-
ear effects is more efficient than the one based on third-order
nonlinearity. Furthermore, the possibility of quasi-phase
matching provides an additional degree of freedom in shift-
ing the comb wavelengths to the targeted center wavelength.
Over the last decade, we have observed a tremendous
development of three-wave mixers based on whispering
gallery resonators. With respect to efficiency at milliwatt
input powers and in terms of compactness they outperform
mirror-based systems. The recent improvements in the fab-
rication of on-chip resonators indicate that efficient and

C 2016 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
I. Breunig: Three-wave mixing in whispering gallery resonators
fully integrated devices will be developed soon and will
also find their way into applications beyond conventional
three-wave mixing.
Acknowledgement. Financial support from the Deutsche
Forschungsgemeinschaft (DFG) is gratefully acknowledged.
Published online: 15 April 2016
Key words: Nonlinear optics, Frequency conversion, Res-
onators.
Ingo Breunig did an apprentice-
ship as a car mechanic. After one
more year working in a garage,
he studied physics at the Uni-
versity of Rostock, and received
his Diploma degree in 2004. He
moved to the University of Bonn
and obtained a Ph.D. in physics in
2009 for a thesis on continuous-
wave optical parametric oscilla-
tors. Then followed a two-year
period as a post-doc. Since 2011,
he leads the research group Non-
linear Optics being part of the Laboratory for Optical Systems
at the University of Freiburg. His current research activities
comprise optical materials, nonlinear-optical phenomena and
whispering gallery resonators.
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