Laser Photonics Rev. 7, No. 3, L17L20 (2013) / DOI 10.1002/lpor.

201200116
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Abstract All optical inscription of quasi phase matching struc-
tures in an x-cut LiNbO
3
crystal is demonstrated. Quasi phase
matching is obtained by periodically lowering the nonlinear re-
fractive index of the crystal using focussed ultrashort pulses.
The structures were used to frequency double 1.55 m light.
The converted signal could be enhanced by a factor of 70 with
respect to the unmodied material. From these measurement
it could be deduced that the nonlinearity has been periodically
damped up to 20%.
Quasi phase matching in femtosecond pulse volume
structured x-cut lithium niobate
Jens Thomas
1,
, Vinzenz Hilbert
1
, Reinhard Geiss
1
, Thomas Pertsch
1
,
Andreas T unnermann
1,2
, and Stefan Nolte
1,2
Within the past years the aim to provide light in any wave-
length regime has driven the eld of nonlinear optics. Appli-
cations range from single frequency sources to broad band
parametric frequency conversion. In most cases, second
order nonlinearities are exploited for sum and difference
frequency generation - with second harmonic generation
(SHG) being the most prominent example.
In many applications, the articial, anisotropic crystal
lithium niobate (LiNbO
3
) is used, which has high nonlin-
ear coefcients. In order to achieve efcient photon con-
version, the phases of the photons of the incident and of the
doubled frequency and 2 have to be matched. Oth-
erwise, back conversion of the second harmonic power
P
2
to the pump P

occurs due to the phase mismatch

k = 2(n
2
n

) /c depending on the difference of re-

fractive indices n

, n
2
at the fundamental and second har-
monic frequency.
Figure 1(a) displays P
2
as a function of propagation
length in the nonlinear medium. All curves have been com-
puted by numerically integrating the coupled-amplitude
equation for a lossless medium [1]. For the case of per-
fect phase matching (k = 0), the dependence is quadratic
(Fig. 1(a), black curve I), for a given mismatch (k = 0),
back conversion starts to occur at the point where the phase
mismatch amounts to (Fig. 1(a), blue curve IV), thus at
a coherence length of
L
c
= /k. (1)
1
Institute of Applied Physics, Abbe Center of Photonics, Friedrich-Schiller-Universit at Jena, Max-Wien-Platz 1, 07743 Jena, Germany
2
Fraunhofer Institute for Applied Optics and Precision Engineering, Albert-Einstein-Str. 7, 07745 Jena, Germany

Corresponding authors: e-mail: thomas@iap.uni-jena.de

In a birefringent crystal, phase matching can be achieved
for conversion of ordinary polarized light to extraordinary
polarized light, by nding an axis of propagation for which
their respective refractive indices are equal. Alternatively,
back conversion can be diminished [2] (Fig. 1, curve III)
or avoided (Fig. 1, curve II) with quasi phase matching
(QPM). Here, the nonlinearity is altered with a period of
2L
c
. Ideally, the sign of the second order nonlinearity d is
reversed (Fig. 1(b), green solid line).
Usually QPM structures are fabricated by means of
electric eld poling, where a high voltage is applied to
the crystal through a patterned masking layer. This tech-
nique is restricted to the d
33
component of the nonlinearity,
consequently just z-cut crystals can be poled such that the
individual domains range through the entire crystal. How-
ever, there are certain applications that require the use of
x-cut crystals, e. g. electro-optic modulators. At the same
time they would benet fromefcient frequency conversion
mediated by QPM. While poling of x-cut crystals has been
demonstrated with surface electrodes, the reversed domains
extended only a few micrometers below the surface [3, 4].
Our aim is to realize a QPM structure that extends far
into the volume of an x-cut LiNbO
3
wafer. Instead of elec-
tric eld poling, we use ultrashort laser pulses to structure
the crystal. This approach has many benets. Most im-
portantly, it is more exible since it does not require any
micro structuring technology to lithographically dene the
respective poling patterns. Additionally, it can easily be
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2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
LASER &PHOTONICS
REVIEWS
L18 J. Thomas et al.: Quasi phase matching in femtosecond pulse volume structured x-cut lithium niobate
Figure 1 Second harmonic power over propagation length (in
units of L
c
) and a sketch of the longitudinal prole of the sec-
ond order nonlinearity d, the solid line displays domain reversal
and the dashed line the investigated periodical lowering of the
nonlinearity.
combined with ultra-short pulse laser based direct writing
of optical waveguides; thus enabling all-optical processing
of integrated optical devices. Several functional elements
could already be demonstrated with the direct write tech-
nique: modulators as well as frequency converters [5] and
most recently Bragg reectors [6]. QPM waveguides how-
ever were only demonstrated in crystals that were poled
already [79]. Mailis et al. demonstrated that the eld of a
femtosecond UV-laser can induce a domain inversion [10].
Albeit, these modications were limited to the surface of
the z-cut sample.
In this paper, we aim not to switch the sign but to peri-
odically lower the nonlinearity by v = d/d
max
as sketched
in Figure 1(b), red dashed line. This approach has been
sucessfully demonstrated on other platforms where domain
poling is not possible, e.g. by reducing the nonlinearity of
GaAs by ion-implantation [2, 11, 12], by Frozen-in eld-
induced second order nonlinearity in optical bers [13] or
more recently in the design of a meta-metarial with a QPM
periodicity [14]. A Fourier transform of the second order
nonlinearity prole yields
d
eff
=
d
max

(1 v) (2)
for the effective second order nonlinearity d
eff
. The ef-
ciency of a QPM structure with lowered nonlinearity is
well below that of a poled one, because back-conversion al-
though reduced is allowed (Fig. 1(a), red dashed curve, III).
Its conversion efciency directly depends on how strongly
the nonlinearity of the crystal is affected by the modi-
cation. Ultrashort pulses can locally alter the crystaline
structure of LiNbO
3
in two ways. They either raise the
Figure 2 Schematic of the sample and inscription setup (a), the
coordinate system is that of the crystal. The inset (b) outlines the
inscription routine of each segment. Inset (c) shows a microscope
image of the endfacet of the QPM structure (inscription pulse
energy of 650 nJ).
extraordinary refractive index (Type I) or destroy the crys-
taline structure, inducing stress elds (Type II) [15]. Two
previous studies addressed how the nonlinearity is affected
within fs written modications. In both a Type I waveguide
had been inscribed in a periodically poled LiNbO
3
and the
decrease of the second order nonlinearity was estimated
by measuring the SHG generated within the waveguide and
comparing it with the numerically calculated conversion ef-
ciency [7,8]. Lee et al. measured a substantially decreased
normalized conversion efciency of 0.0003 %W
1
cm
2
[7], while Osellame et al. achieved 6.5 %W
1
cm
2
and de-
duced that the second order nonlinearity can be conserved
for a certain parameter regime within a Type I modication
[8].
The sample used for the experiments here is a congru-
ent LiNbO
3
wafer, (MgO, 5mol% doped), 0.5 mm thick,
polished as x-cut, with the z-axis of the crystal parallel to
the surface (Fig. 2). The maximum second order nonlinear-
ity d
max
= d
33
can be observed for light polarized along the
z-axis. For pump light of = 2/ =1545 nm, the coher-
ence length L
c
was determined to be 9.5 m [16]. In the
following we assume that the dispersion for the modied
regions is approximately equal and L
c
likewise (see Eq.
(1)). In the pristine crystal, the losses for the fundamental
and second harmonic light were measured to be

= 0.02
dB/cm
2
= 0.05 dB/cm for polarizations parallel to the
z-axis of the crystal.
The structures were inscribed with a cross-bearing
translation stage (Aerotech ALS130, bidirectional repeata-
bility of = 100 nm) and a regenerative amplier (Coher-
ent Reg A, operated at 800 nm, 170 fs pulses, repetition
rate 100 kHz). Its pulse energy could be continously ad-
justed up to 750 nJ with a half wave plate and polarizer
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2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.lpr-journal.org
LETTER
ARTICLE
Laser Photonics Rev. 7, No. 3 (2013) L19
Figure 3 Beamproles of fundamental (a) and second harmonic
light (b), double arrows indicating the direction of polarization. The
coordinate system is that of the crystal.
combination. The light was focussed with a 40 times mi-
croscope objective (NA =0.65) into the sample. We aimed
for a period of = 2L
c
with a lling factor of 0.5. N = 220
periods were realized. For each modied volume, the sam-
ple was translated with a velocity of 1 mm/s as sketched in
the inset of Figure 2. The red part of the arrows indicate
where the shutter of the laser was open. Each of these mod-
ication lines has an elliptical cross-section with a width of
34 m and 1416 m in height. In order to obtain a larger
cross-section of overlapping modications, each modied
region consists of seven vertically overlapping layers of
L = 1 m spaced lines, which are h = 13 m apart.
The nal structure had a cross-section of w = 500 mtimes
h 90 m (Fig. 2(c)). In propagation direction the crystal
was L = 4.6 mm long. The sample was hence character-
ized in a free beam setup. The pump laser was a tunable
laser (Agilent 8164B) combined with an erbiumdoped ber
amplier (EDFA). The system was operated in the pulsed
regime with 40 ns pulses at a 166 kHz rate, delivering a peak
power of 12 W. The light was coupled into the sample with
a lens of 50 mm focal length. Outcoupling was achieved by
a microscope objective (40x, NA=0.65).
In the following we describe the results for the QPM
structure that has been inscribed with 650 nJ pulses.
Although this structures had high propagation losses
(

= 16.4 dB/cm and

2
= 24.5 dB/cm), a signicant
conversion could be obtained. Figure 3 shows the beam
proles of fundamental and second harmonic light after
passage through the QPM structure. Note that both funda-
mental and second harmonic light are polarized parallel to
the z-axis of the crystal, which clearly distiguishes quasi
phase matching from polarization phase matching. While
the beam width is conserved, the beam height of the second
harmonic light is approximately a third of that of the fun-
damental. This indicates that the nonlinearity has not been
modied homogenously over the cross-section. A possi-
ble explanation is that the modication of the non-linearity
follows the same graded prole in the x-direction as the
darkening (Fig. 2c). Thus, the beam size reduction by SHG
is asymmetrically enhanced, because the conversion ef-
ciency is higher in the central region of the structure.
Figure 4 displays the tuning curve at room tempera-
ture. QPM and best conversion is obtained at 1545 nm. For
comparison, the SHG signal of the pristine crystal is also
included (red curve). The conversion efciency could be
Figure 4 Tuning curves for the inscribed QPM structure and the
pristine crystal for comparison.
Figure 5 SHG power vs. input power at the phase matching
wavelength.
enhanced by a factor of up to 70 with respect to the bulk
signal.
Figure 5 shows the power dependence at the phase
matched wavelength. In the structure investigated, we did
not observe saturation due to pump depletion. Thus, the
effective second order nonlinearity can be determined from
the quadratic power law
P
2
= A d
2
eff
P
2

, (3)
where denotes the overal efciency of the QPM structure
and
A =
n

n
2

0
c
4
2
3
L

hF
(4)
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2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
LASER &PHOTONICS
REVIEWS
L20 J. Thomas et al.: Quasi phase matching in femtosecond pulse volume structured x-cut lithium niobate
is a proportionality constant, which depends on the
length of the QPM structure L

= N, a loss term F =
exp ((

+1/2
2
)) and the Boyd-Kleinmann focussing
parameter h = 1.022 (for the focussing conditions within
the experiment) [17, 18]. By inserting the calculated d
eff
and the measured bulk d
33
= 22.49 pm/V in Eq. (2),
we estimated the contrast of the QPM structure to be
v = d/d
max
= 0.82. However, this is an upper limit, since
our estimate assumes = 1 , thus we do not take system-
atic and statistical errors of ll factor and periodicity into
account [19, 20].
QPM structures were also realized with lower and
higher pulse energies, but yielded lower or no conver-
sion. This has two reasons: For low pulse energies, the
induced modication is primarily a positive index change,
which seems to leave the nonlinearity almost untouched
[8]. Higher pulse energies result in a partial darkening
(Fig. 2(c)), which is not only accompanied by a signif-
icant decrease of the second order nonlinearity of up to
20 percent but also by signicantly higher losses. Both fac-
tors have to be balanced to obtain a QPM structure with
good efciency. While the overall conversion efciency is
low compared to z-cut PPLN or surface poled x-cut PPLN
waveguides [3, 4], our approach enables deeply embedding
both modulator and frequency converter on a monolithic
chip. In combination with current research on femtosecond
induced second order nonlinearities in glass [21], QPM
with damping domains might pave the way to truly three-
dimensional nonlinear devices.
Acknowledgements. We like to acknowledge nancial support
by the German Research Foundation (DFG) under priority pro-
gram 1157 and the Leibniz program. Jens Thomas is supported
by the Carl-Zeiss-Foundation.
Received: 5 December 2012, Revised: 30 January 2013,
Accepted: 15 February 2013
Published online: 11 March 2013
Key words: Integrated optics, laser writing, lithium niobate,
nonlinear optics, quasi phase matching.
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