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Physical Review Letters

Raman Generation by Phased and Antiphased Molecular States

Alexei V. Sokolov, D. R. Walker, Deniz D. Yavuz, G. Y. Yin, Stephen E. Harris

Published Jul 17, 2000• 247 citations
Publisher

Abstract

We use molecular deuterium and two driving lasers to demonstrate collinear generation of mutually coherent equidistant sidebands, covering $50000{\mathrm{cm}}^{\ensuremath{-}1}$ of spectral bandwidth and ranging from $2.94\ensuremath{\mu}\mathrm{m}$ to 195 nm in wavelength. The essential idea is the adiabatic preparation of a single, highly coherent ( $|{\ensuremath{\rho}}_{\mathrm{ab}}|\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}0.33$) molecular eigenstate.

DOI
10.1103/physrevlett.85.562

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We use molecular deuterium and two driving lasers to demonstrate collinear generation of mutually coherent equidistant sidebands, covering 50000cm\ensuremath−150000{\mathrm{cm}}^{\ensuremath{-}1}50000cm\ensuremath−1 of spectral bandwidth and ranging from 2.94\ensuremathμm2.94\ensuremath{\mu}\mathrm{m}2.94\ensuremathμm to 195 nm in wavelength. The essential idea is the adiabatic preparation of a single, highly coherent ( ∣\ensuremathρab∣=0.33|{\ensuremath{\rho}}_{\mathrm{ab}}|\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}0.33∣\ensuremathρab​∣=0.33) molecular eigenstate.
Recent experiments have shown that coherent molecular oscillations may generate a comb of coherent collinear sidebands with 50,000 cm/sup -1/ of spectral bandwidth. The essence of this technique is the use of a Raman transition with a sufficiently large coherence that the generation and phase slip length are of the same order. The coherence is established by driving the molecular transition with two single-mode laser fields slightly detuned from the Raman resonance, so as to excite a single molecular superposition state. This talk will summarize the characteristics of this light source and describe two recent experiments which show the mutual coherence of the generated sidebands.
We have demonstrated that coherent molecular modulation can result in the collinear generation of mutually-coherent spectral sidebands that extend in frequency from the infrared to the far ultraviolet. Our technique is based on adiabatic preparation of a highly coherent molecular superposition-state, which is achieved by using narrow-linewidth lasers slightly detuned from a Raman resonance. The phases of the resultant Stokes and anti-Stokes sidebands are adjusted in order to synthesize desired single-cycle pulse trains at the target. In this article we review recent improvements and developments in this area, including: techniques for increasing the number of generated sidebands; synchronization of the pulse trains with the molecular motion in the given molecular system; laser self-focusing and spatial soliton formation due to the coherent interaction of light with oscillating molecules. In the future, this Raman source may produce sub-cycle optical pulses, and allow synthesis of waveforms where the electric field is a predetermined function of time, not limited to a quasi-sinusoidal oscillation.
Parametric Raman sideband generation is investigated using strongly driven Raman coherence in solid hydrogen. We show that the Raman coherence prepared with two coaxial single-mode lasers beats with multimode laser radiation with very broad bandwidth and efficiently replicates the broadband nature to the Raman sidebands without the restriction of phase matching. We demonstrate that this efficient replication occurs mainly on the negative side of Raman detuning, where the medium adiabatically follows the antiphased state.
Detailed numerical modeling of using the vibrational coherence of H2{\mathrm{H}}_{2}H2​ for molecular modulation is presented. The focus of the calculation is on a strongly driven system aimed at producing many sidebands in the presence of Doppler broadening and the effects of collisions at room temperature. It is shown that Dicke narrowing that reduces the Doppler width plays a critical role in high order sideband generation in room temperature H2{\mathrm{H}}_{2}H2​. In addition, the calculation shows that generation of many sidebands favors the phased state as has been reported in all gas phase experiments and is primarily a consequence of the Stark shifts that result from the applied high intensities. The influence of self-focusing in the gas medium that has been conjectured in previous studies is only secondary. The numerical results agree with experimental data obtained in our laboratory, where we have succeeded in generating collinearly propagating Raman sidebands with wavelengths that range from 2216nm2216\phantom{\rule{0.3em}{0ex}}\mathrm{nm}2216nm in the infrared to 133nm133\phantom{\rule{0.3em}{0ex}}\mathrm{nm}133nm in the vacuum ultraviolet. The frequencies covered by these sidebands span over four octaves for a total of more than $70\phantom{\rule{0.2em}{0ex}}600\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$ in the optical region of the spectrum.
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.