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Soviet Journal of Quantum Electronics

Coherent effects in hyper-Raman scattering of a 2nπ pump pulse

Yu. P. Malakyan

Published Apr 30, 1988• 0 citations
Publisher

Abstract

A new effect is predicted in the case of coherent two-photon excitation of a medium consisting of four-level atoms by a 2πn pump pulse: such excitation generates radiation at the hyper-Raman frequency. This takes the form of n successive pulses whose intensity increases toward the trailing edge of the pump pulse.
DOI
10.1070/qe1988v018n04abeh011774

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A theory is developed for transient hyper-Raman scattering and four-wave parametric processes in a gaseous medium subjected to an ultrashort pump pulse field. Investigations are made of the intensity and spectrum of the infrared and ultraviolet radiation generated in a medium as a result of these processes, bearing in mind the transient properties of the pump (phase modulation, pulse profile). It is shown that the initial nonlinearity of the pump field and the parametric processes result in new effects not observed in transient stimulated Raman scattering. For a large two-photon detuning, the hyper-Raman forward scattering is suppressed because of destructive interference with stimulated parametric generation of ultraviolet radiation. The gain of the infrared and ultraviolet radiation depends on the pump pulse profile. Under exact two-photon resonance conditions in the absence of any phase modulation of the pump, infrared and ultraviolet pulses are coherently split into various subpulses and a time-dependent Autler–Townes doublet is observed in their spectrum.
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.
A semiclassical theory of hyper-Raman scattering and three-photon resonant ionization via the coupled density-matrix and Maxwell equations is presented. A simplified three-level atom model is obtained, which includes two-photon resonant pumping and time-dependent photoionization rates. We consider conditions typically encountered in atomic vapors to simulate numerically the pulse propagation. A strong depletion of the photoionization probability in the hyper-Raman field-saturation regime is predicted.
In the presence of coherent saturated near-resonant two-photon excitation, the ordinary Raman scattering line is replaced by a dynamic Stark shifted or Stark split doublet, and Rabi nutations appear in the time-resolved ordinary Raman spectrum. The relative intensity of the peaks of the doublet depends on the shape and on the average frequency of the exciting pulse. Striking new features arise from the interfering contributions of the upper and lower states of the two-photon transition to the Raman scattering process. The theory is applied to Raman scattering in atomic Na in the presence of the 3 2 S 1 2/(F=1, M F =1) to 4 2 D 3 2,5/2/(F=3,M F =3) two-photon resonances.