Two-color pump-probe ionization spectroscopy of gaseous water enhanced by preliminary impulsive Raman excitation

We use sub-10-fs pulses at 400 nm and 15-fs pulses at 800 nm to ionize water molecules and their isotopomers HDO and D₂O in a pump–probe scheme. Pulses are generated via spectral broadening of 25-fs pulses of a 1-kHz Ti:sapphire amplifier system by self-phase modulation in a noble-gas-filled hollow waveguide and subsequent compression using chirped mirrors. At this time scale vibronic excitation of the first bending mode of water in the electronic ground state by impulsive Raman scattering is possible (e.g. the fundamental bending mode of H₂O: t_vib=20 fs). The effect of this pre-excitation on the ionization rate is shown. Received: 14 May 2001 / Revised version: 24 August 2001 / Published online: 19 September 2001     

Intense few-cycle laser pulses from self-compression in a self-guiding filament

Sub-10-fs-pulses are generated by self-compression in a noble gas filament. Using input pulses from a Ti:sapphire amplifier system with an energy of about 1.5 mJ at a repetition rate of 3 kHz and a pulse duration of 30 fs self-compressed sub-10-fs pulses with energies of about 0.3 mJ have been generated. These pulses are characterized with spectral phase interferometry for direct electrical-field reconstruction (SPIDER). Depending on the laser parameters, we observe a significant change in the chirp of the white-light. The spectral distribution of the outcoming beam profile is measured to distinguish the white-light core from the surrounding halo.     

Frequency doubling of phase-modulated femtosecond laser pulses in periodically poled and chirped nonlinear crystals

The second harmonic generation (SHG) at a wavelength of 0.8 μm by 50-and 10-fs pulses with and without phase modulation (PM) was systematically studied in LiNbO₃ crystals with regular domain structure and linearly varied domain thickness. The main results were obtained by numerical method, taking into account the difference between group velocities of interacting pulses and the group-velocity dispersion. In the approximation of the given field of the fundamental radiation, an analytical expression was derived for the spectral density of the second harmonic in the periodically poled nonlinear crystal (PPNC) under nonstationary excitation conditions. It was numerically found that the conversion efficiency of about 90% can be achieved by doubling the frequency of 50-fs laser pulses without PM in the LiNbO₃ PPNC. The maximum conversion efficiency for the SHG by PM pulses is achieved at a certain optimum chirp step in the crystal domain length, which depends on both the value and sign of frequency modulation.     

High repetition rate Q-switched microchip Nd:YVO4 laser with pulse duration as short as 1.1 ns

We have demonstrated a compact and an efficient passively Q-switched microchip Nd:YVO₄ laser by using a composite semiconductor absorber as well as an output coupler. The composite semiconductor absorber was composed of an LT (low-temperature grown) In_0.25Ga_0.75As absorber and a pure GaAs absorber. To our knowledge, it was the first demonstration of the special absorber for Q-switching operation of microchip lasers. Laser pulses with durations of 1.1 ns were generated with a 350 μm thick laser crystal and the repetition rate of the pulses was as high as 4.6 MHz. The average output power was 120 mW at the pump power of 700 mW. Pulse duration can be varied from 1.1 to 15.7 ns by changing the cavity length from 0.45 to 5 mm. Pulses with duration of 1.67 and 2.41 ns were also obtained with a 0.7 mm thick laser crystal and a 1 mm thick laser crystal, respectively.     

Generation of fs laser pulses from a ps pulse-pumped optical parametric amplifier with a beat-wave seed signal

We describe a method of ultrashort-pulse and ultrafast-pulse-train generation through optical parametric amplification of a laser beat wave. Numerical simulation shows that 250-fs laser pulses at 1.55 μm are generated from a beat-wave seeded optical parametric amplifier pumped by a 30-ps laser at 1064 nm. The pulse compression is attributable to sideband generation and parametric amplification under group velocity mismatch. Our experimental result confirms efficient generation of comb-like sidebands for the mixing waves from such an optical parametric amplifier.     

Sum frequency generation of continuously tunable blue pulses from a two-branch femtosecond fiber source

We report on the generation of femtosecond blue pulses from a two-branch mode-locked erbium-doped fiber source. This is achieved by sum-frequency mixing in β-barium borate between the frequency doubled laser radiation at 770 nm and a tunable near-infrared component generated inside a highly nonlinear fiber. Small angle tuning of the nonlinear crystal leads to a continuously variable output wavelength in the visible band between 460 nm and 500 nm. Average power levels exceeding 1.5 mW were collected throughout the entire tuning range of our device, which delivered sub-300-fs pulses at a repetition rate of 98 MHz. These values indicate that the input near-infrared radiation is up-converted with a photon efficiency of 20%.     

Compact sub-100-fs Nd:silicate laser

We present a compact Nd:silicate laser pumped by a single 1-W high-brightness commercial laser diode that generates pulses as short as 88 fs (nearly Fourier limited) when passively mode-locked with a saturable absorber mirror. We also tested a prismless cavity setup employing a single Gires-Tournois mirror, yielding 100-fs pulses. These setups are significantly simpler and more compact than those reported previously for short pulse Nd:silicate lasers.     

Sum and difference frequency generation of white light continuum with the ps pulses of Nd:YAG laser in a thick BBO crystal

The white light continuum (WLC) generated in water/D₂O mixture by pumping with the fundamental of ps Nd⁺³:YAG laser has been used as a variable frequency source for the sum frequency generation as well as for its amplification. 35 ps long pulses with 8 mJ energy at 1064 nm were mixed collinearly with the WLC generated by the same laser beam in a 20 mm thick BBO crystal. The obtained tunable output has been identified as the sum frequency between the fundamental and a portion of the WLC with the required phase matching. Theoretical simulations are also given along with a few initial experiments to use this combination for the difference frequency generation (optical parametric amplification) under non-collinear geometry.     

Highly efficient frequency doubling of high-energy Nd:YAG laser using a CsB3O5 crystal

We have demonstrated efficient frequency doubling of high-energy fundamental Nd:YAG laser pulse energy of the multi-joule (J) level at a high repetition rate using high optical-quality top-seeded solution growth CsB₃O₅(TSSG-CBO) crystal for the first time. Second-harmonic (532 nm) generation (SHG) output energy of 1.2 J at 10 Hz is obtained with a conversion efficiency of 60%. This result has been obtained at the multi-J level by the growth of high optical-quality TSSG-CBO crystal with the large effective nonlinear coefficient and high damage threshold. These results indicate that TSSG-CBO is a good candidate material for high-energy SHG of Nd-doped lasers at the several J level or more with high repetition rate.     

Broadband four-wave optical parametric amplification in bulk isotropic media in the ultraviolet

We report on four-wave optical parametric amplification of the ultrashort ultraviolet light pulses in bulk fused silica and CaF₂. Exact phase-matching in these isotropic media is achieved by means of non-collinear interaction with cylindrical beam focusing. Four-wave optical parametric amplifier efficiently operates in the UV spectral range with 1-ps laser pulses, delivering amplified signal energy exceeding 50 μJ using millijoule pump pulses in the visible (527 nm). Results of scanning of the parametric gain profile suggest that broad amplification bandwidth as wide as ∼20 nm (at FWHM) under these experimental settings is achieved, which might support amplification of sub-10-fs ultraviolet pulses with central wavelength around 330 nm. It is also shown experimentally and verified theoretically that the parametric gain profile exposes a distinct inhomogeneity and its bandwidth notably broadens due to effects of self- and cross-phase modulation imposed by the intense pump beam.     

High-peak power multi-wavelength picosecond pulses generated from a BaWO4 Raman-seeded optical parametric amplifier

We report the generation of high-peak power multi-wavelength picosecond laser pulses using optical parametric amplification (OPA) in BBO seeded with pulses generated in a 5-mm length BaWO₄ crystal by stimulated Raman scattering of 18-ps laser pulses at 532 nm. The maximum output energy of the amplified first-Stokes component at 559.7 nm was about 1.76 mJ. The corresponding maximum peak power, pulse duration and spectral line width were measured to be 117.3 MW, 15 ps and 18.0 cm⁻¹, respectively. The multi-wavelength picosecond laser pulses were in the visible and near infrared ranges. Using this Raman-seeded OPA technique, the beam quality of the stimulated Raman scattering pulses can be improved.     

Simple electro-optic technique to generate temporally flat-top laser pulses

A simple technique is presented to generate temporally flat-top shaped laser pulses using electro-optic modulator (Pockels cell). It involves splitting of input laser pulse into two halves of equal intensity and then stacking together with appropriate optical delay to get a temporally flat-top laser pulse. It also allows generation of other pulse shapes by varying the relative intensity, delay, and phase between two halves of the input laser pulse. Temporally flat-top laser pulses of duration ~ 9 ns have been generated using ~ 7 ns duration incident laser pulses from a flash lamp pumped Q-switched Nd:glass laser oscillator. The rise and fall-time of the shaped pulse is limited by speed of electro-optic switch (Pockels cell), which is ~ 2 ns in the present case.     

Second harmonic generation by femtosecond Yb-doped fiber laser source based on PPKTP waveguide fabricated by femtosecond laser direct writing

The frequency doubling of femtosecond pulses from an Yb-doped fiber laser source was demonstrated in a PPKTP waveguide fabricated by femtosecond laser direct writing. The PPKTP waveguide contains a fixed period of 8.9 μm and the feomtosecond fundamental pulses have a central wavelength of 1044 nm. A maximum SHG power of 406 mW was produced, yielding a conversion efficiency of 5.6%. Numerical simulations were carried out to investigate the property of frequency doubling for femtosecond pulses. The results show that the SHG process proceeds even the quasi-phase-matching (QPM) condition is not well satisfied, which is significantly different from that of “long” pulses or CW light and is accorded with the experimental results.     

Generation of sub-6-fs blue pulses by frequency doubling with quasi-phase-matching gratings

We demonstrate the generation of sub-6-fs pulses centered at 405 nm by frequency doubling of 8.6-fs Ti:sapphire laser pulses. The frequency doubling is carried out in a nonlinearly chirped quasi-phase-matching grating fabricated in a lithium tantalate substrate. This device simultaneously provides frequency conversion and pulse compression of the positively prechirped fundamental pulses. The second-harmonic pulses are characterized in a cross-correlation setup, and their pulse shapes are retrieved by two iterative phase-reconstruction algorithms. The generated second-harmonic spectrum spans a bandwidth of 220 THz. To our knowledge, these are the shortest pulses ever generated in the blue spectral region.     

Self-starting five optical cycle pulse generation in Cr<Superscript>4+</Superscript>:YAG laser

We report stable self-starting near-transform-limited 26-fs pulses at 250-mW output power from a Kerr-lens mode-locked (KLM) Cr⁴⁺:YAG laser using chirped mirrors in combination with prisms. The highest output power achieved in KLM regime was 600 mW at 55-fs pulse duration. The experimental results agree well with the results of theoretical analysis with respect to KLM self-starting ability and stability against continuous-wave and multi-pulse operation. Parameter ranges for stable transform-limited KLM pulses as well as the shortest achievable pulse durations are established. Using an InGaAs-InP semiconductor saturable absorber mirror we could obtain self-starting 57-fs pulses at the average output power of 200 mW. Two-photon absorption was found to be the main mechanism favoring the multiple-pulse operation. Received: 2 May 2002 / Revised version: 16 July 2002 / Published online: 8 January 2003 RID="*" ID="*"Corresponding author. Fax: +43-1/58801-38799, E-mail: sorokina@tuwien.ac.at     

Characterization of Ag and Au nanoparticles created by nanosecond pulsed laser ablation in double distilled water

Pulsed laser ablation of Ag and Au targets, immersed in double-distilled water is used to synthesize metallic nanoparticles (NPs). The targets are irradiated for 20 min by laser pulses at different wavelengths—the fundamental and the second harmonic (SHG) (λ = 1064 and 532 nm, respectively) of a Nd:YAG laser system. The ablation process is performed at a repetition rate of 10 Hz and with pulse duration of 15 ns. Two boundary values of the laser fluence for each wavelength under the experimental conditions chosen were used—it varied from several J/cm² to tens of J/cm². Only as-prepared samples were measured not later than two hours after fabrication. The NPs shape and size distribution were evaluated from transmission electron microscopy (TEM) images. The suspensions obtained were investigated by optical transmission spectroscopy in the near UV and in the visible region in order to get information about these parameters. Spherical shape of the NPs at the low laser fluence and appearance of aggregation and building of nanowires at the SHG and high laser fluence was seen. Dependence of the mean particle size at the SHG on the laser fluence was established. Comments on the results obtained have been also presented.     

Generation of 15 W femtosecond laser pulse from a Kerr-lens mode-locked Yb:YAG thin-disk oscillator

We demonstrated a robust power-scalable Kerr-lens mode-locked(KLM) operation based on a Yb:YAG thin-disk oscillator.15-W,272-fs pulses were realized at a repetition rate of 86.7 MHz with an additional Kerr medium and a 2.5 mm hard aperture in the cavity.247-fs pulses with an average power of 11 W could also be obtained by using a 2.4 mm hard aperture.Based on this shorter pulse,high efficient second-harmonic generation(SHG) was performed with a 1.7-mm-long Li B3O5(LBO) crystal.The SHG laser power was up to 5 W with the power fluctuation RMS of 1% measured over one hour.     

Intra-cavity second harmonic generation with Nd:YVO4/BIBO laser at 542 nm

We report, for the first time, an efficient intra-cavity second-harmonic generation (SHG) at 1084 nm in a nonlinear optical crystal, BiB₃O₆(BIBO) at the direction of (θ, ?) = (170.1°, 90°), performed with a LD end-pumped cw Nd:YVO₄ laser. With 590 mW diode pump power, a continuous-wave (cw) SHG output power of 19 mW at 542 nm yellow-green color has been obtained using a 1.5 mm-thick BIBO crystal. The optical conversion efficiency was 3.22%. It was found that the output wavelength could be 532 nm, 537 nm or 542 nm according to regulating the angle of BIBO.     

Specialty Yb fiber amplifier for microchip Nd laser: Towards ∼1-mJ/1-ns output at kHz-range repetition rate

We demonstrate and optimize, for a mJ/ns release at the wavelength 1.064 μm, the operation of a compact laser system designed in the form of a hybrid, active-passive, Q-switched Nd³⁺:YAG/Cr⁴⁺:YAG microchip laser seeding an Yb-doped specialty multi-port fiber amplifier. As the result of the amplifier optimization, ∼1 mJ, ∼1 ns, almost single-mode pulses at a 1-10-kHz repetition rate are achieved, given by a gain factor of ∼19 dB for an 11-μJ input from the microchip laser. Meanwhile, a lower pulse energy, ∼120 μJ, but a much higher gain (∼25 dB) are eligible for the less powerful (0.35 μJ) input pulses.     

A three-wavelength Ti:sapphire femtosecond laser for use with the multi-excited photosystem II

We have constructed a three-wavelength Ti:sapphire femtosecond laser with an independent tunable wavelength (λ₁) and two variable central wavelengths (λ₂ and λ₃) for use with the multi-excited photosystem II. Stable sub-40-fs pulses are generated. The λ₁-wavelength pulses can be tuned independently from 750 nm to 850 nm. The center wavelengths λ₂ and λ₃ can be varied from 760 nm to 840 nm. Received: 14 April 2000 / Revised version: 5 September 2000 / Published online: 27 April 2001