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Conference on Lasers and Electro-Optics

Parametric four-wave mixing in strongly driven Raman molecular gas

Aurélien Benoît, Benoît Beaudou, Benoît Debord, Frédéric Gérôme, Fetah Benabid

Published Jan 1, 2016• 0 citations
Publisher

Abstract

We propose and demonstrate parametric four-wave mixing in a Raman active gas. Two lasers with a 1.7 THz frequency-difference in a strongly-driven Raman rotational-transition of D2 generate sidebands with frequency-spacing equal to the lasers frequency-difference.
DOI
10.1364/cleo_si.2016.sw1p.4

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Four-wave optical parametric amplification (FWOPA) in a Raman-active medium is experimentally investigated by use of an air-filled hollow fiber. A femtosecond pump pulse shorter than the period of molecular motion excites the coherent molecular motion of the Raman-active molecules during the parametric amplification of a signal pulse. The excited coherent motion modulates the frequency of the signal pulse during the parametric amplification, and shifts it to lower frequencies. The magnitude of the frequency redshift depends on the pump intensity, resulting in intensity-dependent spectral characteristics that are different from those in the FWOPA induced in a noble-gas-filled hollow fiber.
The explicit solution is obtained for Raman four-wave mixing ω4=ω1−ω2+ω3\omega_4=\omega_1-\omega_2+\omega_3ω4​=ω1​−ω2​+ω3​ of two strong fields E1,E3E_1, E_3E1​,E3​ and two weak fields E2,E4E_2, E_4E2​,E4​ in a four-level system with the large Doppler broadening. The resonance of the mixing coefficient vs intensity is found near equal Rabi frequencies of strong fields and interpreted as an intersection of quasi-energy levels. Up to 6 peaks appear in the dependence of conversion coefficient on the detuning of the probe field. An unexpected additional pair of peaks is a result of averaging over velocities and disappears at low temperature. The effects allow explaining saturation behavior in recent experiments on the mixing in sodium molecular vapor.
We report an experimental observation of simultaneous rotational and vibrational collinear Raman generation in low pressure cooled deuterium gas, with only two narrow-band laser pulses applied at the input of the molecular cell. Only the fundamental vibrational transition Q1{Q}_{1}Q1​ (0) is driven strongly in this experiment. However, in addition to efficient vibrational Raman generation we observe generation of a large number of rotational sidebands (more than 100) corresponding to S0{S}_{0}S0​ (0) transition. We notice that fine-tuning of the frequency difference of the driving fields near the vibrational Raman resonance changes dramatically the aspects of the generated spectrum and the efficiency of rotational generation: from complete suppression of a self-starting stimulated rotational Raman generation to a strong enhancement of two orders of magnitude. We conduct a numerical analysis that allows us to attribute this behavior to quantum interference among the probability amplitudes of the three molecular states involved.