Efficient 1 kHz femtosecond optical parametric

amplification in BiB3O6 pumped at 800 nm

Masood Ghotbi and Majid Ebrahim-Zadeh
ICFO-Institut de Ciencies Fotoniques, Mediterranean Technology Park,08860 Castelldefels, Barcelona, Spain

Valentin Petrov, Pancho Tzankov and Frank Noack

Max-Born-Institute for Nonlinear Optics and Ultrafast Spectroscopy, 2A Max-Born-Str. D-12489 Berlin, Germany
petrov@mbi-berlin.de

Abstract: We demonstrate efficient operation of a tunable femtosecond

optical parametric amplifier based on BiB3O6 pumped at 800 nm by a 1 kHz
Ti:sapphire regenerative amplifier. The idler wavelength coverage extends
to beyond 3 µm and the pulse duration at this wavelength is of the order of
110 fs. This new nonlinear borate crystal offers exceptionally high
nonlinearity, making it a very promising candidate for power scaling of such
frequency converters in the near-IR.
©2006 Optical Society of America
OCIS codes: (190.4970) Parametric oscillators and amplifiers; (190.4400) Nonlinear optics,
materials; (190.7110) Ultrafast nonlinear optics.

References and links

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bismuth borate BiB3O6 (BIBO),” Solid State Commun. 109, 249-251 (1999).
2. Zh. Lin, Zh. Wang, C. Chen, and M.-H. Lee, “Mechanism for linear and nonlinear optical effects in
monoclinic bismuth borate (BiB3O6) crystal,” J. Appl. Phys. 90, 5585-5590 (2001).
3. H. Hellwig, J. Liebertz, and L. Bohaty, “Linear optical properties of the monoclinic bismuth borate
BiB3O6,” J. Appl. Phys. 88, 240-244 (2000).
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optical parametric oscillation and third harmonic generation in the new nonlinear optical material BiB3O6,”
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Washington, DC 2002), paper CWA27, pp.232-233.
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(BiB3O6) optical parametric oscillators,” Appl. Phys. B 80, 55-60 (2005).
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BiB3O6,” Conference on Lasers and Electro-Optics CLEO 2006, OSA Technical Digest CD-ROM (OSA,
Washington, DC 2006), paper JThC64.
7. M. Ghotbi, A. Esteban-Martin, and M. Ebrahim-Zadeh, “BiB3O6 femtosecond optical parametric
oscillator,” Opt. Lett. 2006 (In Press).
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symmetry,” Appl. Opt. 44, 6971-6985 (2005).
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Varanavicius, “Highly efficient parametric conversion of femtosecond Ti:sapphire laser pulses at 1 kHz,”
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growth, thermal and optical performance of BiB3O6,” J. Cryst. Growth 233, 282-286 (2001).
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#74151 - $15.00 USD Received 16 August 2006; revised 27 September 2006; accepted 5 October 2006
(C) 2006 OSA 30 October 2006 / Vol. 14, No. 22 / OPTICS EXPRESS 10621
1. Introduction
Bismuth triborate, BiB3O6 (BIBO), is an interesting and relatively new nonlinear optical
crystal belonging to the borate family. Its main advantage is the exceptionally high second
order nonlinear susceptibility [1] which is associated with the contribution of the BiO4 anionic
group [2]. The effective nonlinearity of BIBO can be larger than that of KTP and the lower
transparency edge extends deeper into the UV (286 nm) [3]. High nonlinear coefficients are
an important prerequisite for realization of down-converting optical parametric devices in
which the required pump intensities to achieve the threshold are often so high that damage
problems occur (optical parametric oscillators, OPOs, travelling-wave type optical parametric
generators, OPGs, and optical parametric amplifiers, OPAs) or in which the parametric gain,
when using unamplified pump sources, is extremely low, as is the case in, for example,
synchronously pumped OPOs (SPOPOs). There exist only very few demonstrations of the
down-conversion potential of BIBO. The first report [4] on BIBO-based nanosecond OPO
operation with pumping at 532 nm and the subsequent extension of this work with pump
sources at different repetition rates [5] revealed greater potential of BIBO in comparison to
KTP, BBO, and LBO. OPG/OPA operation of BIBO at 10 Hz in the picosecond regime was
demonstrated only very recently, with 35 ps pump pulses also at 532 nm [6]. BIBO was
implemented also in a SPOPO operating at 76 MHz although in this case the purpose was to
produce femtosecond pulses in the visible and the pumping was at 400 nm [7].
All previous down-conversion experiments confirmed the good damage resistivity of
BIBO which is related to its band-gap. In addition, the fact that the band-gap is below 300 nm
makes this crystal very suitable for pumping with short pulses in the 800 nm spectral range,
using Ti:sapphire laser systems, because two-photon absorption can be avoided. In this work
we investigate the potential of BIBO as an OPA for such down-conversion from the 800 nm
spectral range into the near-IR, by using amplified femtosecond pulses at 1 kHz as a pump.
2. Phase-matching properties of BIBO for OPA
Although initially several different set-up configurations and also different crystals were
tested, the material now in use for near-IR OPGs/OPAs, and in particular in commercial
devices, with 800 nm pumping, is type-II BBO [8]. This is due to several important
advantages the most important of which is the possibility to tune, even close to degeneracy,
with almost constant signal and idler bandwidth. The bandwidth is determined basically by
the group velocity mismatch (GVM) between the signal and idler pulses. As a monoclinic
crystal with point group 2, BIBO is optically biaxial which offers a greater variety of phase-
matching configurations. Nevertheless, for the same reason, it is preferable to use type-II
interaction and for a pump wavelength of 800 nm this is possible only in the x-z principal
plane where BIBO can be regarded as optically positive (oe-o or eo-o interaction).9 For these
processes the effective nonlinearity, assuming a signal wavelength of 1400 nm, is
deff=d12cosθ≈2.4 and ≈2.2 pm/V, respectively [9], see Fig. 1(a). This means that the nonlinear
figure of merit, which involves also the index of refraction, of BIBO is roughly two times
higher than that of BBO.
As can be seen from Fig. 1(a), the tunability for oe-o interaction is achieved with much
smaller angle variation than for eo-o interaction. In addition, the spectral bandwidth defined as
the absolute value of the GVM parameter, 1/vS-1/vI, is larger and less dependent on the
wavelength in the former case. Thus, type oe-o interaction is preferable for BIBO exactly as in
the optically negative BBO where eo-e interaction possesses such properties. These two cases
are compared in Fig. 1(b). It can be seen that BIBO, similar to BBO, exhibits for a pump
wavelength of 800 nm the property that the signal and idler waves travel in opposite directions
relative to the pump which ensures exponential growth of the parametric gain even beyond the
pulse walk-off length [10]. However, as can be expected from the smaller band-gap, the GVM
of BIBO is larger, i.e. the spectral acceptance per unit length is smaller. Thus shorter crystals
should be used in the femtosecond regime which compensates for the larger effective
nonlinearity. Nevertheless, the use of shorter crystals helps to avoid undesirable higher order

#74151 - $15.00 USD Received 16 August 2006; revised 27 September 2006; accepted 5 October 2006
(C) 2006 OSA 30 October 2006 / Vol. 14, No. 22 / OPTICS EXPRESS 10622
nonlinear processes and to better utilize the transparency window of a given crystal. Since in
the case of down-conversion the limiting factor is the mid-IR cut-off edge it can be expected
that shorter crystals of BIBO will permit wider tunability. Indeed, idler absorption limits the
tunability with BBO to less than 3 µm, e.g. max. 2.7 µm in Ref. [11], or even less (2.5 µm) in
commercial devices. On the other hand the 3 µm spectral range is very important for
molecular spectroscopy. The transmission problem can be circumvented by employing other
non-borate crystals such as KTP in a second stage but it is difficult to produce short pulses
with them [12].

3.0

signal and idler wavelengths [nm]

4000
o BIBO, Type-II, x-z plane (a)
2.5
3500

3000 2.0

deff [pm/V]
2500 1.5

2000 1.0
1500
0.5
1000 e
0.0
35 40 45 50 55 60 65 70 75 80 85 90
polar angle θ [°]

200
BIBO: oe-o (b)
BBO: eo-e BIBO
100
GVM [fs/mm]

BBO

-100
1/vP-1/vI
1/vS-1/vI
-200
1000 1100 1200 1300 1400 1500 1600
signal wavelength [nm]

Fig. 1. Angle tunability and effective nonlinearity deff of BIBO in the x-z optical plane (oe-o
and eo-o interaction) for a pump wavelength of 800 nm (a), and comparison of the GVM
parameters 1/vP-1/vI and 1/vS-1/vI for BIBO (oe-o) and BBO (eo-e), where vP, vS, and vI denote
the pump, signal, and idler group velocities.

For the present experiment, two uncoated samples of BIBO were available, both cut at
θ=42° in the x-z optical plane, with an aperture of 7×7 mm2 and thicknesses of 3 and 5 mm.
The transparency measured for polarization parallel to the y principal optical axis (o-
polarization with respect to the x-z plane) is shown in Fig. 2. If compared to the first
measurements in Ref.3, it can be seen that the substructure below 2.5 µm is in fact absent in
the present crystals. The spectra, in particular the long-wave edge, are very similar to those
measured in Ref. [13]. The transparency is indeed better for the thinner crystal. Comparing
with BBO [14], one can conclude that although the absolute upper limits for the transmission
are similar, for the same thickness, BBO exhibits an absorption feature below 2.5 µm.

#74151 - $15.00 USD Received 16 August 2006; revised 27 September 2006; accepted 5 October 2006
(C) 2006 OSA 30 October 2006 / Vol. 14, No. 22 / OPTICS EXPRESS 10623
 100
E//y
80

transmission [%]
60

40

20
BIBO (5 mm)
BIBO (3 mm)
0
300 400 2000 2500 3000 3500
wavelength [nm]

Fig. 2. Transparency of the used BIBO samples for polarization parallel to the y principal
optical axis corresponding to the pump and idler waves.

3. Experimental results
We compared BIBO and BBO in a modified set-up of a commercial double-pass OPA seeded
by white light continuum (Clark-MXR), shown in Fig. 3. The continuum is generated in a 2-
mm thick sapphire plate which is simultaneously used to adjust the proper polarization. A
polarizer between the two passes through the nonlinear crystal serves to select the signal
wavelength for seeding the second pass. The pump energy used to pump the second pass was
300 µJ. Finally, the signal and idler pulses are coupled out using a mirror slightly displaced in
the uncritical direction.

Ti:sapphire laser oscillator and amplifier

500 µJ, 80 fs, 1 kHz, 800 nm

delay 375 µ J

T BS
L
BS WLG
L
delay
T

P DM OPA DM
DM 800 nm
CM
output

Fig. 3. Experimental set-up of the seeded OPA: L, lenses, T, telescopes, BS, beam splitters,
DM, dichroic mirrors, CM, curved mirror with 30 cm radius of curvature, WLG, white light
continuum generation, OPA, optical parametric amplifier.

Using a standard BBO crystal which was 5 mm thick but antireflection-coated, the
tunability extended from 1180 to 2500 nm with a maximum output level of 80 µJ
(signal+idler) for a pump energy of 375 µJ. Such overall conversion efficiencies (of the order
of 20%) are typical for tunable femtosecond OPGs/OPAs based on BBO type-II crystals [11].

#74151 - $15.00 USD Received 16 August 2006; revised 27 September 2006; accepted 5 October 2006
(C) 2006 OSA 30 October 2006 / Vol. 14, No. 22 / OPTICS EXPRESS 10624
The 5-mm long BIBO crystal provided more output energy than the 3-mm long BIBO crystal,
but the temporal and spectral characteristics were not satisfactory: depending on the
wavelength, the signal and idler pulses were either structured or longer than 200 fs as a result
of the pulse splitting and reconversion. Thus it can be concluded that the larger GVM in
BIBO, see Fig. 1(b), requires the use of shorter crystals than in the case of BBO.

50 200

40 180

pulse energy [µJ]

pulse duration [fs]

30 160

140
20
120

100
10
1000 1500 2000 2500 3000 3500
wavelength [nm]

Fig. 4. Pulse energy (full squares) and pulse duration (FWHM) assuming Gaussian pulse
shapes (full circles) for the BIBO based OPA using a 3-mm thick sample. The open triangles
show the energy obtained with the standard antireflection-coated 5-mm thick BBO crystal.

With the 3-mm thick BIBO crystal, we were able to obtain sub-200 fs pulse duration
throughout the whole tuning range (Fig. 4). The pulse duration was estimated by fitting cross
correlation traces obtained by sum-frequency generation with a reference pulse at 800 nm
using a 0.7 mm thick type-I BBO crystal. Gaussian pulse shapes were assumed and the time-
bandwidth product was estimated by measuring the pulse spectra with a multichannel analyzer
equipped with a 128-element pyroelectric array. In principle the range of the pulse durations
obtained with the 3-mm thick BIBO was similar to the results with the standard 5-mm thick
BBO crystal, but the dependence on the wavelength was different. The shorter signal and idler
pulse durations obtained in the limits of the tunability range of BIBO (Fig. 4) can be explained
by the increasing acceptance bandwidth, see Fig. 1(b).

1.0
1.0

0.8
intensity [a.u.]

155 nm
0.5
0.6
136 fs

0.4 0.0
2800 3200
wavelength [nm]

0.2

0.0

-800 -400 0 400 800

delay [fs]

Fig. 5. Cross correlation trace of the idler pulses at 3050 nm obtained by sum-frequency
generation with a reference pulse at 800 nm (black symbols) and a Gaussian fit (red line). The
inset shows the corresponding idler spectrum.

The main advantage of BIBO seems the possibility to have somewhat larger tuning range
extending to slightly above 3 µm, while under the same conditions the tuning with BBO had
an upper limit of ≈2.5 µm, Fig. 4. Although the maximum energy level obtained with BIBO

#74151 - $15.00 USD Received 16 August 2006; revised 27 September 2006; accepted 5 October 2006
(C) 2006 OSA 30 October 2006 / Vol. 14, No. 22 / OPTICS EXPRESS 10625
was of the same order of magnitude (80 µJ for signal+idler), the internal conversion efficiency
was obviously higher (more than 30% in the maximum for the second pass) because this
sample was uncoated.
Figure 5 shows a cross-correlation function of the idler pulses at 3050 nm (black symbols)
from the FWHM of which (136 fs) a pulse duration of 110 fs is obtained by a fitting
procedure (red curve). The time-bandwidth product is 0.55, somewhat above the Fourier limit
of 0.44 for Gaussian pulse shapes (it is ≈0.5 for the pump pulses). The pulses at the signal
wave (1085 nm) are slightly shorter having a FWHM of 100 fs.
4. Summary and Conclusion
In summary, we have implemented for the first time to our knowledge the BIBO crystal in a
800 nm pumped femtosecond optical parametric amplifier and demonstrated efficient and
tunable operation with certain advantages (extension to the 3 µm spectral range) in
comparison to BBO. The shortest pulses obtained were of the order of 100-110 fs. Another
practical advantage in comparison to BBO, which is at present the standard material for this
application, is the non-hygroscopicity of BIBO. Similar results with type-II BIBO pumped
near 800 nm can be expected also in the picosecond regime. On the other hand, preliminary
analysis indicates that type-I interaction in BIBO can be quite useful for generation and
amplification of broad femtosecond continua. Work is in progress to investigate other phase-
matching configurations with BIBO for this application and to scale the output energy by
using large aperture crystals.
Acknowledgment
We acknowledge financial support from the EU within Laserlab Europe (contract RII3-CT-
2003-506350).

#74151 - $15.00 USD Received 16 August 2006; revised 27 September 2006; accepted 5 October 2006
(C) 2006 OSA 30 October 2006 / Vol. 14, No. 22 / OPTICS EXPRESS 10626