Second - harmonic generation of ultra-high

intensity femtosecond pulses with a KDP crystal

M. Aoyamaa, T. Harimotob, J. Maa, Y. Akahanea and K. Yamakawaa
a
Advanced Photon Research Center, Kansai Research Establishment,
Japan Atomic Energy Research Institute,
Umemidai 8-1, Kizu, Kyoto 619-0215, Japan.
Phone: +81-774-71-3327, Fax: +81-774-71-3316,
E-mail: yamakawa@apr.jaeri.go.jp
b
Faculty of Engineering, Yamanashi University, Takeda 4-3-11, Kofu, Yamanashi 400-8511,
Japan

Abstract: We investigated second harmonic generation with ultrahigh

intensity femtosecond laser pulses from a terawatt Ti: sapphire laser system.
Energy conversion efficiency of about 80 % for a type I potassium
dideuterium phosphate crystal was obtained with 130 fs laser pulses at an
intensity as high as 192 GW/cm2.
2001 Optical Society of America
OCIS codes: (140.7090) Ultrafast lasers; (190.2620) Frequency conversion

References and links

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9. Y. Tamaki, M. Obara and K. Midorikawa, " Second harmonic generation from intense, 100-fs Ti Sapphire
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generation and wave-front correction of a terawatt laser system," Opt. Lett. 25, 508-510 (2000).
12. T. Ditmire, A. M. Rubenchik, D. Eimerl, and M. D. Perry, "Effects of cubic nonlinearity on frequency
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41(2002).

#37246 - $15.00 US Received October 18, 2001; Revised November 14, 2001
(C) 2001 OSA 19 November 2001 / Vol. 9, No. 11 / OPTICS EXPRESS 579
1. Introduction
Since the appearance of chirped pulse amplification (CPA) laser systems, there has been
rapid progress in generating high peak power, ultrashort laser pulses. Such lasers can realize
pulses with a peak intensity of >1020 W/cm2 [1] and are therefore useful for a variety of high-
field applications such as the generation of ultrafast x-ray radiation [2] and high harmonic
generation [3] from solid targets. In general the ultrashort laser pulses from a CPA laser
system have amplified spontaneous emission (ASE) background associated with the main
laser pulse and pre- and post-pulses. In a laser - matter interaction experiment, such pre-
pulses and ASE would create a low density plasma in advance of the main laser pulse and
thus significantly alter the physics of the laser - matter interaction [4]. It is significantly
important for the study of the high field laser - solid target interaction experiments.
Frequency conversion of femtosecond pulses can improve intensity contrast of laser pulses.
Simple experimental configuration of second-harmonic generation (SHG) and improvement
of intensity contrast are so attractive for some applications of intense femtosecond laser
pulses. However it is well known that there are problems [5-6] in frequency conversion such
as SHG with sub-picosecond and femtosecond laser pulses. The effectiveness of the SHG
with ultrashort laser pulses can be greatly reduced by group-velocity mismatch between the
fundamental and generated second harmonic (SH) pulses. At high intensities the local
refractive index of the crystals changes with the laser intensity, primarily because of the third-
order nonlinear susceptibility, resulting in phase modulation and self-focusing effects. These
effects will also influence the conversion efficiency and pulse duration of the SH pulse. In
order to reduce effects of the dispersion and the higher-order nonlinear processes, a crystal
with a thin thickness is generally necessary.
A number of groups have investigated SHG with intense femtosecond laser pulses with
intensities exceeding ~100 GW/cm2. Chien et al. [7] reported an energy conversion efficiency
of 80 % for 4 mm thick type I potassium dideuterium phosphate (KDP) crystals using 500 fs,
1053 nm laser pulses at an intensity as high as 400 GW/cm2. Krylov et al. [8] investigated
SHG of type I KDP crystals with crystal lengths of 3, 5, 10, and 40 mm, respectively, using
150 fs, 780 nm laser pulses at an intensity as high as 150 GW/cm2. They concluded that
energy conversion efficiency could not exceed 50 % due to the modulation of the phase of the
fundamental pulses. Tamaki et al. [9] described SHG of intense femtosecond pulses using
three types of crystals. They obtained an energy conversion efficiency of approximately 20 %
for a 1 mm thick type I KDP crystal and for a 1 mm thick type I cesium lithium borate
(CLBO) crystal using 100 fs, 800 nm laser pulses at intensities as high as 200 GW/cm2 and
30 GW/cm2, respectively. Neely et al. [10] investigated frequency conversion of intense
picosecond laser pulses with 4 mm and 2 mm long KDP crystals. They observed the break-up
of the far field of the SH pulse due to the thickness of the crystal and the high intensity. More
recently, Queneuille et al. [11] discussed SHG and wavefront correction for high intensity
laser pulses with a deformable mirror. They obtained an energy conversion efficiency of
approximately 55 % for a 4 mm thick type I KDP crystal and using 400 fs, 1053 nm laser
pulses at an intensity as high as 200 GW/cm2. They estimated an obtained intensity contrast
of ~109 with SHG.
As we mentioned above, frequency conversion with picosecond or sub-picosecond laser
pulses accomplished more than 50% efficiencies. However conversion efficiencies with ~100
fs laser pulses are lower than those with sub-picosecond laser pulses. As Krylov et al. [8]
pointed out, energy conversion efficiency should be lower than 50 % using thick crystals with
150 fs laser pulses. They showed that phase modulation of the fundamental pulses decreases
the frequency conversion efficiency for intensities less than 150 GW / cm2. Ditmire et al. [12]

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numerically discussed the precompensation for a phase shift due to the third-order
susceptibility χ(3) by affording an initial phase mismatch upon the doubling crystal on SHG
with ultrahigh intensity laser pulses. Their calculated results on some experimental conditions
showed the possibility for obtaining an energy conversion efficiency of about 70 - 80 % with
ultrahigh intensity laser pulses of ~100 fs and incorporating this precompensation into their
calculations.
In order to obtain higher conversion efficiency, we investigated SHG with fundamental
laser pulses of ~100 fs in more than the hundreds of GW / cm2 intensity regime with a
technique of the precompensation described by Ditmire et al.. Although frequency conversion
of sub-picosecond laser pulses with thick crystals enables high efficiency conversion, the
thick crystals degrade the beam quality of SH pulses. In our experiment a thin crystal was
used for SHG in order to reduce effects of dispersion, beam-breakup and third-order
nonlinear processes. This method with intense femtosecond pulses also makes the
experimental arrangement of frequency conversion simple. Therefore, it is easy to apply to
any kind of CPA laser system.
In this paper, we describe frequency conversion with a thin crystal and ~100 fs high
intensity laser pulses from a terawatt Ti: sapphire laser system. We have achieved an energy
conversion efficiency of about 80 % for a type I KDP crystal with 130 fs laser pulses for
intensities as high as 192 GW/cm2 and have found no optical fatal damage of the nonlinear
crystal.

2. Experimental setup
We used a part of our Ti: sapphire CPA laser system [1] in this study. The system is seeded
with pulses from an all-solid-state mirror-dispersion-controlled Ti: sapphire oscillator capable
of producing 10-fs pulses. These pulses are temporally stretched by a factor of 100,000 in an
all-reflective, cylindrical mirror-based pulse expander. Then, stretched pulses are amplified
with two amplifier stages. The Ti: sapphire amplifier chain consists of a regenerative
amplifier, and a four-pass amplifier. These amplifiers are pumped by a fraction of the 532 nm
radiation at 10 Hz from Q-switched Nd: YAG lasers. We also controlled the central
wavelength and spectral bandwidth of amplified pulses using angle-tuned thin etalons in the
regenerative amplifier. Then, the Ti: sapphire amplifier chain laser pulses are compressed
with a parallel grating pair which uses 1200 lines/mm. The intensity of the fundamental
pulses can be adjusted by using the half-wave plates and thin film polarizers before the
compressor. The compressed pulses have a spectral width of 14.7 nm at full-width at half
maximum (FWHM) and a center wavelength of 800 nm. The output pulse duration used in

Pulse
L1 compressor
SM

C1 f=1 m
PM1

DM KDP crystal SM
SM
C2 DM
L2
Spectrometer SM SM
PM2

Fig.1: Experimental setup for SHG with femtosecond laser pulses. SM: silver mirror, DM: dichroic mirror, PM1:
power meter for

aser pulses
L1: lens for SH laser pulses, C1: CCD camera for SH laser pulses, PM2:
power meter for fundamental laser pulses, L2: lens for fundamental laser pulses, C2: CCD camera for
fundamental laser pulses.

#37246 - $15.00 US Received October 18, 2001; Revised November 14, 2001
(C) 2001 OSA 19 November 2001 / Vol. 9, No. 11 / OPTICS EXPRESS 581
this experiment was about 130 fs.
The optical layout of SHG is depicted in Fig. 1. The fundamental pulses were focused
with a 1000 mm focal-length concave mirror on a SHG crystal. SHG was achieved in the
Type I 1-mm-thick KDP crystal which has a sol-gel antireflective coating and a transmission
spatial quality of λ / 7.5 @ 800 nm. The crystal was positioned 56 cm away from the focusing
mirror. The laser pulses focused on the KDP crystal had an elliptical shape with a major
diameter of 5.76 mm and a minor diameter of 2.73 mm. The generated SH and fundamental
pulses were separated with a dichroic mirror. Spectral properties of the dichroic mirror were
calibrated with a spectrophotometer (U-400, Hitachi Ltd.). Images of the SH and fundamental
pulses were taken with charge-coupled device (CCD) cameras that were placed after the
nonlinear crystal. We observed the images of a point on the nonlinear crystal.

3. Experimental and numerical results

Experimental and numerical energy conversion efficiencies of the fundamental laser
intensities from 0 to 500 GW/cm2 are shown in Fig. 2 and Fig. 4. The energy of the
fundamental and generated SH pulses was measured with a power meter (PE - 10 and PE-25,
Ophir Optronics Inc.). All experimental points were obtained by averaging over 300 laser
pulses. The conversion efficiency was corrected for loss from the mirrors and the KDP

Fig. 2: Experimental and numerical energy conversion efficiencies of SHG as a function of fundamental
intensity. Circles indicate experimental results. The solid curve shows the numerical result where the
calculation includes a phase shift due to the third-order susceptibility χ(3). The dot curve shows the numerical
result of the SH pulse duration.

crystal. The experimental results and the calculated results are shown in Fig. 2. This
calculation model is based on the set of coupled equations describing the propagation of the
fundamental and SH pulses, which includes a frequency chirp, group velocity mismatch,

#37246 - $15.00 US Received October 18, 2001; Revised November 14, 2001
(C) 2001 OSA 19 November 2001 / Vol. 9, No. 11 / OPTICS EXPRESS 582
group velocity dispersion of the fundamental and the SH pulses. These equations also take
other physical effects into account : a phase shift due to the third-order susceptibility χ(3),
second-order nonlinear susceptibility [13]. This numerical result in Fig.2 was obtained for
fundamental pulses which had no frequency chirp. The experimental energy conversion
efficiency was about 80 % at the intensity of 192 GW/cm2. The calculated and experimental
results of the energy conversion efficiency behave similarly. Although pulse duration of the
generated SH pulses were not measured, the calculated result shows the SH pulse duration
was shorter than the pulse duration of the fundamental pulses at 192 GW/cm2. At this
intensity the broadening of the SH spectrum was not observed with self-phase modulation as

Fig.3: Measured spectra of second harmonic pulses. The solid curve and the dot curve show the SH
spectrum at an intensities of the fundamental pulses as high as 219 GW/cm2 and 455 GW/cm2,
respectively.

shown in Fig.3. Therefore, we conjecture that such phase modulation doesn’t almost affect
the SH pulse duration at the optimum intensity of the energy conversion efficiency. We had
however observed spectral broadening of SH pulses due to self-phase modulation in the more
than ~230 GW /cm2.
On the other hand, a calculated energy conversion efficiency with fundamental pulses
which have an appropriate frequency chirp is shown in Fig.4. When the fundamental pulses
have an appropriate frequency chirp, this method can also be used to shift the laser intensity
for optimum conversion efficiency towards the more than ~500 GW / cm2 intensity regime
and at the same time suppress the effect of the third-order susceptibility. However
undesirable frequency chirp of the fundamental pulses reduces the energy conversion
efficiency. We found this case in Fig.4. The experimental fundamental pulses in Fig.4 had a
positive group delay dispersion of 6.06 × 102 fs2/nm. The experimental conversion efficiency
decreases to 60 %. We also found that the laser intensity for optimum conversion efficiency
depends on the initial frequency chirp of the fundamental laser pulse. Beyond the optimum
laser intensity the conversion efficiency decreases. The phase shift due to χ(3) causes this
phenomenon. This means that the optimum laser intensity can be controlled with the initial
phase shift such as by the frequency chirp of the fundamental laser pulse or the initial phase
mismatch[13].

#37246 - $15.00 US Received October 18, 2001; Revised November 14, 2001
(C) 2001 OSA 19 November 2001 / Vol. 9, No. 11 / OPTICS EXPRESS 583
 The measured far-field profile of the SH pulse at a fundamental intensity of about 190
GW/cm2 indicates that the spatial quality of the SH laser pulse and the fundamental pulses are
1.3 and 1.1 times diffraction limited, respectively. The results show that the thin crystal

Fig.4: Experimental and numerical energy conversion efficiencies of SHG as a function

of the fundamental intensity. Circles indicate experimental results. The solid and dot
curves show the numerical results where the calculation includes a phase shift due to
the third-order susceptibility χ(3) and a frequency chirp of 6.18× 104 fs2/nm and 3.24 × 104
fs2/nm, respectively.

suppresses degradation of the beam quality at even high fundamental intensity. It should be
noted that we have found no optical fatal damage of the KDP crystal from CCD images of the
laser pulses.
This SHG does not require a complicated experimental setup, so it leads to higher
efficiency. This method is suitable for SHG of a large CPA system, which generates >100 fs
and > TW laser pulses. Under this condition, SHG can also be achieved without temporal
broadening of the SH pulses. As mentioned in Section 1, Queneuille et al. [11] discussed
SHG and wavefront correction. They obtained an energy conversion efficiency of
approximately 55 % for a 4 mm thick type I KDP crystal using 400 fs, 1053 nm laser pulses
at an intensity as high as 200 GW/cm2. They obtained pulses which had focused intensity of 4
x 1019 W/cm2 with estimated intensity contrast of ~109 with SHG and a deformable mirror.
The thickness of the KDP crystal in our experiment is thinner than that on above experiment.
sThe thin crystal can suppress degradation of the beam quality compared with thick crystals.
Therefore, frequency conversion of intense femtosecond pulses can improve the intensity
contrast of laser pulses to some degree even without a deformable mirror. It is important for
the study of high intensity laser - matter interaction. The simple experimental configuration
of this SHG and improvement of intensity contrast are very attractive for some applications
of intense femtosecond laser pulses. Furthermore, as mentioned in Ref. 13, an initial
frequency chirp of the fundamental pulse in SHG with ultrahigh intensity laser pulses can be
used to suppress third-order nonlinearity in the temporal and spatial profile. This method can

#37246 - $15.00 US Received October 18, 2001; Revised November 14, 2001
(C) 2001 OSA 19 November 2001 / Vol. 9, No. 11 / OPTICS EXPRESS 584
also be used to shift the laser intensity for optimum conversion efficiency towards the more
than ~500 GW / cm2 intensity regime and at the same time suppress the degradation of the
beam quality. At the expense of pulse broadening we obtain higher beam quality of the
generated SH pulses and accomplish SHG with a smaller aperture of the laser pulse during
the frequency conversion stage by the frequency chirp of the fundamental pulses. In a
preliminary calculation, we found that a frequency chirp of the fundamental pulses can
suppress the spectral broadening of SH pulses when SHG is accomplished in the more than
~500 GW / cm2 intensity regime. These ultrahigh intensity laser pulses enable a smaller
aperture of the laser pulse during the frequency conversion stage. So this SHG method can
also be accomplished in a smaller aperture nonlinear crystal. This leads to a higher
transmission spatial quality of the crystal, compared with a large aperture crystal. The crystal
used in this experiment has a clear aperture of about 40 mm in diameter. We can expect that
the fundamental pulses of 5.8 TW at 470 GW/cm2 can be converted into SH pulses of 4.4 TW
with this crystal.

4. Conclusion
We have investigated second harmonic generation with ultrahigh intensity femtosecond laser
pulses from a terawatt Ti: sapphire laser system.  The maximum energy conversion
efficiency was about 80 % at a laser intensity of 192 GW/cm2 without optical damage of the
type-I KDP crystal. SHG with intense femtosecond pulses makes experimental arrangements
of frequency conversion simple. This method can also be used to shift the laser intensity for
optimum conversion efficiency towards the more than ~500 GW / cm2 intensity regime and at
the same time suppress the degradation of the beam quality. At the expense of pulse
broadening we obtain higher beam quality and accomplish SHG with a smaller aperture of the
laser pulse during the frequency conversion stage. Furthermore, this can be accomplished
with a smaller aperture nonlinear crystal. Therefore, it is feasible to apply this method to any
kind of CPA laser system.

Acknowledgment
The authors would like to thank Professor M. Nakatsuka of ILE, Osaka University for
providing us with a KDP crystal and Y. Inoue, H. Ueda and A. Sagisaka for their technical
support. The authors are also thankful to Dr. James K. Koga for many helpful comments.

#37246 - $15.00 US Received October 18, 2001; Revised November 14, 2001
(C) 2001 OSA 19 November 2001 / Vol. 9, No. 11 / OPTICS EXPRESS 585