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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

High-efficiency generation of high-order harmonics in intense laser fields with coherent Raman self-scattering

I. P. Prokopovich, A. A. Khrutchinsky

Published May 6, 1996• 0 citations
Publisher

Abstract

The dynamics of high-intense laser fields at coherent Raman self-scattering are investigated by the use of numerical simulation. The processes under investigation take place at the Raman scattering on electronic states in atoms with transition to be forbidden in electro-dipole approximation, on vibrational or rotational states in molecules, on states connected with the spin flip and other. It is found that the threshold intensities exist provided that the pulse duration is smaller than dephasing time of the Raman transition in the medium. Under this, the following processes occur: an effective generation of the high-order harmonics comes up; the plateau forms in the harmonic spectrum. The maximum which arises on this plateau shifts to the higher-harmonic numbers in case of the higher threshold intensities of the pulse. It is shown how the transformation of the initial pulse intensity into high-order harmonics intensity can be considerably increased with the different initial parameters of the pulse and the medium.

DOI
10.1117/12.239740

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The dynamics of high-intense laser fields at coherent Raman self-scattering are investigated by the use of numerical simulation. The processes under investigation take place at the Raman scattering on electronic states in atoms with transition to be forbidden in electro-dipole approximation, on vibrational or rotational states in molecules, on states connected with the spin flip and other. It is found that the threshold intensities exist provided that the pulse duration is smaller than dephasing time of the Raman transition in the medium. Under this, the following processes occur: an effective generation of the high-order harmonics comes up; the plateau forms in the harmonic spectrum. The maximum which arises on this plateau shifts to the higher-harmonic numbers in case of the higher threshold intensities of the pulse. It is shown how the transformation of the initial pulse intensity into high-order harmonics intensity can be considerably increased with the different initial parameters of the pulse and the medium.
High order Raman generation has received considerable attention as a possible method for generating ultrashort pulses. A large number of Raman orders can be generated when the Raman-active medium is pumped by two laser pulses that have a frequency separation equal to the Raman transition frequency. High order Raman generation has been studied in the different temporal regimes, namely: adiabatic, where the pump pulses are much longer than the coherence time of the transition; transient, where the pulse duration is comparable to the coherence time; and impulsive, where the bandwidth of the ultrashort pulse is wider than the transition frequency. To date, almost all of the work has been concerned with generating as broad a spectrum as possible, but we are interested in studying the spectra of the individual orders when pumped in the transient regime. We concentrate on looking at extra peaks that are generated when the Raman medium is pumped with linearly chirped pulses. The extra peaks are generated on the low frequency side of the Raman orders. We discuss how linear Raman scattering from two-photon dressed states can lead to the generation of these extra peaks.
The coherent scattering spectrum of a three-level atom driven by an intense laser field with multiphoton resonant excitation is considered. The spectrum corresponding to harmonic generation is investigated both analytically and numerically for different initial atomic states. The analytical calculations are based on the generalized rotating wave approximation, which allows one to explain obtained spectra containing in general both even and odd harmonics. The results applied to the hydrogen atom show that one can achieve efficient generation of moderately high harmonics using multiphoton resonant excitation by appropriate laser pulses.
We have investigated the behavior of high-order stimulated Raman scattering in a highly-transient regime. We demonstrate efficient collinear generation of vibrational sidebands in molecular hydrogen and methane using two-color pumping with pulses of duration $\ensuremath{\tau}\ensuremath{\sim}100\phantom{\rule{0.3em}{0ex}}\mathrm{fs}$ tuned to a vibrational Raman transition. A Raman spectrum with a large bandwidth was observed, ranging from the IR to the UV. Under some conditions strong pump depletion was observed and up to five anti-Stokes sidebands were observed to have energies exceeding 10% of the transmitted pump pulse energies. A numerical simulation reproduces qualitatively and quantitatively the experimental results and allows us to explain key experimental features. The simulation also confirms that the molecular coherence in the medium is substantially increased by the two-color pumping and allows us to deduce values for the degree of material excitation. The use of this technique looks promising for efficient subfemtosecond pulse generation.
We suggest that subfemtosecond pulses can be generated by using high-order stimulated Raman scattering when a Raman transition is driven by three intense single-mode laser beams with two different modulation frequencies. An oscillatory strong Raman coherence is established by the modulated molecular modulation. Numeric simulations based on the first fundamental vibrational Raman transition of gaseous and solid deuterium indicate that subfemtosecond pulses can be generated by Raman excitations with above, below, or opposite Raman detunings.
Saturation of vibrational Raman coherence and coherent anti-Stokes Raman scattering (CARS) using femtosecond (fs) excitation pulses is investigated theoretically. The pump in a typical fs-CARS configuration has a bandwidth of a few hundred cm${}^{\ensuremath{-}1}$ that can couple tens of rotational states of room-air nitrogen molecules simultaneously, unlike in CARS with longer pulse durations. It is demonstrated that the vibrational coherence and also the vibrational CARS with fs excitation display saturationlike behavior once the rotational coherence is saturated. The Raman saturation threshold for the fs pump is numerically estimated to be at a peak intensity of $\ensuremath{\sim}$1022{10}^{22}1022 W/m2{}^{2}2, which is six to seven orders of magnitude higher than that in the nanosecond regime. The results are compared with the known saturation thresholds in different pulse-duration regimes and placed in perspective with other nonlinear thresholds reported in fs excitation regimes.
We present the most prominent features in two-colour coherent control of high-order harmonic generation using a strongly driven two-level atom model, which are known to generate high harmonics as well as hyper-Raman lines with a plateau and a cut-off. Furthermore, for one laser field case, we find, when the hyper-Raman lines are located at the position of the high harmonics, that the high harmonics are strongly enhanced due to the interference effect between the high harmonics and the hyper-Raman lines. Within these conditions, by combining the laser field with another much weaker laser field, we show plentiful and strong high harmonics in the light spectrum of the driven atomic system.