Generation of high-order rotational lines by four-wave Raman mixing using a high-power picosecond Ti:Sapphire laser

More than thirty rotational lines equally spaced by 587 cm^–1 are generated simultaneously in the vicinity of the fundamental line by four-wave Raman mixing using a high-power picosecond Ti:Sapphire laser as a pump source and hydrogen as a Raman medium. Since the wavelength of this multifrequency laser emission extends from the near-infrared to the near-ultraviolet, it can be utilized as a tunable light source for picosecond spectroscopy. Because of the wide spectral bandwidth available, this procedure has great potential for the generation of ultrashort laser pulses by mode-locking these emission lines.     

Infrared degenerate four-wave mixing and resonance-enhanced stimulated Raman scattering in molecular gases and free jets

2 H₂), methane (CH₄), carbon dioxide (CO₂), and nitrous oxide (N₂O) in a cell under equilibrium conditions and cooled in free jet expansions. For methane at room temperature the detection limit was 2×10¹² molecules per cm³ and quantum state, enabling the detection of trace species with a spatial resolution of 1 mm²×30 mm. In an attempt to study transitions in the ν₁+ν₃ and 2ν₂+ν₃ combination bands of CO₂ or N₂O, it was not possible to observe any DFWM signal. Instead a surprisingly strong, backward- and forward-directed emission was found which could not be attributed to the DFWM process. The signal arising from this emission was more than 2 orders of magnitude stronger than the DFWM signals obtained for other molecules. The frequencies of the emitted radiation were found to correlate with the transitions ν₁+ν₃→ν₁ and 2ν₂+ν₃→2ν₂, respectively. Our investigations lead to the conclusion that the emission can be explained by stimulated Raman scattering, resonantly enhanced by transitions to the combination levels ν₁+ν₃ and 2ν₂+ν₃. This process seems to suppress the generation of DFWM signals. Received: 1 October 1996/Revised version: 6 January 1997     

Generation of more than 40 rotational Raman lines by picosecond and femtosecond Ti:sapphire laser for Fourier synthesis

Received: 14 November 1996     

Efficiently generated rotational and vibrational stimulated raman emission by means of a two-color laser beam

When a two-color laser beam is introduced into pressurized hydrogen, about 40 laser emission lines are generated from the ultraviolet to the visible regions. This phenomenon is ascribed to the stimulated Raman effect due to a combination ofJ=1 J=3 rotational andv=0 v=1 vibrational transitions. By introducing the two-color laser beam, the threshold for generation of the rotational line is substantially reduced. The present phenomenon is attributed to four-wave mixing, which allows efficient generation of higher-order rotational and vibrational Raman lines.     

VUV generation by frequency tripling the third harmonic of a picosecond kHz Nd:YLF laser in xenon and mercury vapour

uv ^vac=351.165 nm) of a ps 1 kHz Nd:YLF laser system is frequency tripled in xenon and mercury vapour. About 4×10⁴ photons per pulse, i.e. 4×10⁷ photons/s, are generated in xenon yielding a conversion efficiency of η=3×10^-10. The unusual frequency tripling in xenon takes place in a positive dispersive wavelength region. It is shown that Kerr-induced dispersion in the atomic system and a fifth-order process rather than a third-order process can explain the frequency tripling. For comparison a four-wave mixing process is investigated in negative dispersive mercury vapour. Due to absorption of the generated VUV radiation in the autoionization region of mercury the observed effective efficiency is, in our experimental arrangement, even lower than in xenon. An analysis of the VUV generation with respect to absorption is given. Received: 1 September 1997     

Generation of more than 40 laser emission lines from the ultraviolet to the visible regions by two-color stimulated raman effect

An intense and monochromatic laser beam consisting of more than 40 vibrational and rotational lines is generated by the stimulated Raman effect, when two-color laser beams separated by 590 cm^–1 are tightly focused into pressurized hydrogen. This phenomenon is reasonably explained by four-wave mixing; one beam is used for two-step excitation (₁+₁) to an imaginary level and another beam (₂) acts as a seed beam, generating a fourth beam (2₁–₂). Through cascade processes, so many laser emissions appear with a frequency difference of (₁–₂) in entire ultraviolet and visible regions.     

Effect of partial coherence on four-wave mixing in photorefractive materials via reflection grating approximation

We investigate the effect of beam coherence on four-wave mixing via reflection gratings in photorefractive media. For the case of phase conjugation, the results of our theoretical analysis indicate that partial coherence always leads to a drop of signal gain and phase conjugate reflectivity in non-depleted cases. In general, the mutual coherence of the signal beam and the pump beam can be enhanced due to the process of wave mixing. The mutual coherence of the phase conjugate beam and one of the pump beams depends on the beam intensity ratio as well as the optical path difference. This is distinctly different from the four-wave mixing case with a transmission grating. Received: 15 October 1999 / Revised version: 26 June 2000 / Published online: 7 February 2001     

Study of non-linear optical phase conjugation in Ca by resonant degenerate four-wave mixing via bound excited states

. The dependence of the reflectivity on the vapour density, the buffer gas pressure and the pump beams intensity was investigated. The influence of the strong linear absorption was taken into account in a theoretical model that led to a satisfactory interpretation of the experimental results. A maximum reflectivity of 46% was measured under optimized conditions. The effect was also studied through the high-lying bound states . The maximum measured reflectivity was as high as for the first excited state. The effect of the oscillator strength on the reflectivity was demonstrated experimentally and interpreted with the help of a simple theoretical model. Received: 11 June 1996     

Quasi-rotational spectral structure of optical radiation due to stimulated Raman scattering and parametric processes in high-pressure hydrogen

Received: 20 June 1997/Revised version: 26 January 1998     

Parametric four-wave mixing in the 3d and 4d Rydberg states of NO

2 Σ⁺,H^′ 2Π^±(v^′=2), and 4dσ,πO²Σ⁺,O^′ 2Π^±(v^′=0) Rydberg states of NO molecules are described. The analyses of the two-photon excitation functions and infrared emission spectra revealed that only the ²Π^- component was involved in PFWM. This is in good accordance with the absence of amplified spontaneous emission (ASE) in the ²Σ⁺ and ²Π⁺ components due to their predissociative character. Results provide some support for the mechanism that the generation of the vacuum ultraviolet radiation was brought by PFWM in which ASE served as a third driving wave. Received: 6 January 1998     

Generation of UV and VIS laser light by stimulated Raman scattering in H2, D2, and H2/He using a pulsed Nd:YAG laser at 355 nm

2 ), deuterium (D₂), and mixtures of hydrogen and helium (H₂/He), versus Raman gas pressure and input pump energy of the pulsed Nd:YAG laser at 355 nm, are reported. Photon conversion efficiencies of 50% and 27% are achieved at the first Stokes lines (S₁) in H₂ and D₂, respectively. As a result, ultraviolet and visible laser light (274–503 nm) was generated with energies ranging from a few mJ up to several tens of mJ. Received: 5 January 1998/Revised version: 3 June 1998     

Thermal grating and broadband degenerate four-wave mixing spectroscopy of OH in high-pressure flames

2 ∑–X²Π(0,0) band of OH has been studied in premixed methane/air flames using a cw Ar⁺ laser probe. Measurements of flame temperature and pressure were derived from fits of theoretical simulations to the observed time variation of signals over a pressure range of 10 to 40 bar and for different stoichiometry that were in agreement with independent measurements using N₂ CARS and predictions of a one-dimensional flame calculation. Broadband DFWM spectra in the same band of OH were observed up to a pressure of 9 bar, above which signals were obtained only from scattering from thermal gratings. Received: 10 November 1997/Revised version: 28 May 1998     

Experimental study with a Fourier set-up of the image transfer from a laser beam to a forward or backward stimulated Raman scattered beam

Received: 13 July 1998 / Revised version: 8 October 1998 / Published online: 24 February 1999     

N2 laser frequency conversion by stimulated Raman scattering in H2

High-efficiency frequency conversion in H₂ of a nitrogen laser oscillator-amplifier system is described. The laser system provides about 1 MW output power with a very low intrinsic divergence. Up to 3 Stokes lines at 392, 468, and 581 nm and 3 Anti-Stokes at 296, 263, and 237 nm, respectively, have been observed at the output of the 60 cm long H₂ Raman cell. Peak power values of 500, 300, and 70 kW have been measured for the first 3 Stokes, respectively, corresponding to a 56% pump energy conversion efficiency.A comparison between free and guided propagation (in a hollow dielectric waveguide) is also reported, for various values of the pump intrinsic divergence.     

Analysis of degenerate four-wave mixing spectra of NO in a CH4/N2/O2 flame

4 /N₂/O₂ flame to spectral simulations based on a two-level theory for stationary, saturable absorbers by Abrams et al. Temperatures determined from least-squares fits of simulations to experimental spectra in the A²Σ⁺?X²Π⁺(0,0) band are compared to temperatures obtained from OH absorption spectroscopy and a radiation-corrected thermocouple. We find that DFWM rotational temperatures derived from Q-branch spectra agree with thermocouple and are independent of pump laser intensity for low to moderate saturation (I≈I_sat). However, the temperatures are systematically low and depend on pump intensity if the analysis neglects saturation effects. We demonstrate a method for obtaining an effective pump saturation intensity for use with the two-level model. This approach for analyzing saturated DFWM line intensities differs from previous work in that the use of the theory of Abrams et al. rather than a transition-dipole-moment power law allows treatment of a much wider range of saturation. Based on the observed signal-to-noise ratio an NO detection sensitivity of 25 ppm is projected, limited by a DFWM background interference specific to hydrocarbon flames. Received: 15 September 1998 / Revised version: 18 November 1998 / Published online: 24 February 1999     

Parametric four-wave mixing in the H2Σ+,H′2Π(v′=0) states of NO

2 Σ⁺,H^′2Π(v^′=0)←X²Π(v^′′=0) two-photon transition of NO, both near-infrared and vacuum ultraviolet radiation were emitted along the laser propagation direction. The analyses of emission and excitation spectra revealed that the parametric four-wave mixing (PFWM) process coexisted with amplified spontaneous emission. Polarization properties of the IR radiation are found to be dependent on the rotational levels. Pressure and laser power behaviors of the generated waves were reported. The mechanism of PFWM was discussed in terms of selection rules of the relevant ro-vibronic transitions. Received: 19 September 1996/Revised version: 27 January 1997     

Experimental investigation of the effect of collisions and temperature on degenerate four-wave mixing

An experimental investigation (including a comparison with a simple theoretical model) of the effect of buffer-gas composition, pressure and temperature on resonant Degenerate Four-Wave Mixing (DFWM) has been performed. The DFWM signal from NO in a quartz cell was measured and the effect of quenching as well as elastic (phase-changing) collisions was studied by varying the total and partial pressures of N₂ and CO₂ as buffer gases. It was found that the DFWM signal first slowly increased with buffer-gas pressure (up to 10 mbar) and then rapidly decreased. It was furthermore found that the DFWM signal was considerably less sensitive to quenching collisions as compared to Laser-Induced Fluorescence (LIF) (for laser intensities approximately equal to half the DFWM saturation intensity of the transition). On the other hand, while LIF is virtually insensitive to elastic collisions, DFWM displays a larger sensitivity to elastic collisions than to quenching collisions. The DFWM saturation intensity was found to increase with buffer-gas pressure (although slower than expected). When varying the temperature of the gas composition, it was found that the DFWM signal decreased markedly with increasing temperature. This decrease is too fast to be explained solely by a change in the population of the molecular state probed by the laser.     

Detection of oxygen atoms in a high pressure surfatron microwave discharge via two-photon four-wave mixing

3 P_J) oxygen atoms are detected in a high pressure surface wave discharge driven at 2.45 GHz via two-photon resonant degenerate four-wave mixing spectroscopy (TP-DFWM) in the forward folded BOX configuration. The nonlinear optical signal provides a direct measure of the relative oxygen atom concentration with high spatial resolution inside the discharge up to pressures of 1 bar and without distortions due to linear absorption or saturation effects. The axial distribution of oxygen atom concentration is observed to depend sensitively on total pressure and gas flux. For total gas pressures up to 600 mbar both in case of a mixture of 10% O₂/He and 10% O₂/Ar the concentration of oxygen atoms increases linearly with pressure. At higher pressures an increase with larger slope is observed for 10% O₂/Ar, while the concentration remains constant for 10% O₂/He. This is interpreted by an increase of the three-body recombination rate in O₂/He mixtures. Received: 26 July 1996/Revised version: 15 November 1996     

Excited-state absorption and stimulated emission of tetrahedral Co2+ ion in LiGa5O8

Differential absorption spectra measurements of tetrahedral Co²⁺-doped LiGa₅O₈ have been made using a ps pump-probe technique. The stimulated emission from the ⁴T₁(⁴P) level to the ⁴A₂(⁴F) and ⁴T₂(⁴F) states is observed to be overlapped by the excited-state absorption. The excited-state absorption is tentatively assigned to transition from the ⁴T₁(⁴P) level of the Co²⁺ ion to the conduction band of LiGa₅O₈. For Co²⁺:LiGa₅O₈, laser operation is expected to be possible in the vicinity of 720 nm and in the 860–970 nm spectral region. Received: 5 June 1998 / Revised version: 20 October 1998 / Published online: 19 May 1999