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Quantum Electronics

Temporal dynamics of parametric transformation in a Raman-active medium with the induced rotational coherence

Anatolii V Andreev, Anton A. Valeev, Viacheslav B. Morozov, A. N. Olenin, Vladimir G. Tunkin

Published Jan 31, 2002• 2 citations
Publisher

Abstract

The collinear generation of radiation with a multicomponent spectrum is obtained upon scattering of picosecond pulses in gaseous hydrogen coherently excited by the pulsed biharmonic pump in resonance with the Raman-active rotational S 0 (1) transition. Probe pulses at 355 nm were almost completely transformed to the radiation with the multicomponent spectrum of width ~5000 cm -1 and the components spaced by 587 cm -1 . The solution of a system of equations for the four-photon Raman — parametric interaction is obtained in the plane-wave dispersionless approximation in the spectral and time representations. The equations describe the transformation of probe pulses in gas with the induced coherence into an arbitrary number of interacting spectral components. The consideration performed in the second order of the dispersion theory provides good agreement with experiments on the transformation into different spectral components depending on the probe-pulse delay.

DOI
10.1070/qe2002v032n01abeh002126

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The collinear generation of radiation with a multicomponent spectrum is obtained upon scattering of picosecond pulses in gaseous hydrogen coherently excited by the pulsed biharmonic pump in resonance with the Raman-active rotational S 0 (1) transition. Probe pulses at 355 nm were almost completely transformed to the radiation with the multicomponent spectrum of width ~5000 cm -1 and the components spaced by 587 cm -1 . The solution of a system of equations for the four-photon Raman — parametric interaction is obtained in the plane-wave dispersionless approximation in the spectral and time representations. The equations describe the transformation of probe pulses in gas with the induced coherence into an arbitrary number of interacting spectral components. The consideration performed in the second order of the dispersion theory provides good agreement with experiments on the transformation into different spectral components depending on the probe-pulse delay.
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.
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.
Optical nutation at the Raman-active transition 6P 1/2−6P 3/2 of thallium atoms (ω R /2πc=7793 cm −1) under resonant Raman excitation by a biharmonic picosecond pulsed field, giving rise to substantial motion of the population, is detected. Optical nutation appears as an oscillatory behavior of the energy of the anti-Stokes scattering of probe pulses, which follow with a fixed delay, as a function of the product of the energies of the excitation pulses. As a result of the dynamic Stark effect, which decreases the frequency of the transition under study, resonance excitation conditions are satisfied for negative initial detunings of the Raman excitation frequency from resonance. The Raman scattering cross section for the transition under study is estimated by comparing the experimental data with the calculations.
Abstract The theory of multifrequency stimulated Raman scattering (SRS) of light on rotational transitions of molecules, which are simulated by a three-level quantum system, is developed. It is shown that the application of bichromatic pumping increases the scattered radiation spectrum width. The exact algebraic solution for the wave amplitudes is obtained in the simplest version of synchronous SRS on transitions with a negligibly low eigenfrequency. It is found that an increase in the ratio of the Raman transition frequency to the pump radiation frequency leads to predominance of the anti-Stokes scattering branch. The effect of wave asynchronism emerging due to linear and nonlinear dispersion of the medium as well as the phase difference of the pump waves on SRS is considered. All types of asynchronism narrow generated frequency spectrum and suppress the anti-Stokes scattering branch. Nonlinear dispersion ensures positive values of wave amplitudes due to phase jumps by π during the propagation of waves in a medium.
The solid para-hydrogen film was prepared by depositing the para-hydrogen vapor onto a sapphire substrate. From the stimulated Raman scattering experiment using two ns-lasers whose laser-frequency difference is equal to the fundamental vibrational transition of the solid para-hydrogen, we observed the collinear generation of Raman sidebands. The high-order Raman sidebands were obtained under the strong pumping intensity (≥230 MW/cm 2 ). The generated five anti-Stokes(AS)-Raman sidebands extend from ultraviolet (292 nm for AS 5 band) to visible (565 nm for AS 1 band) region. Also, we found that the first AS-Raman signal shows weak rotational components as well as a strong vibrational line. From the experiment that makes the multimode probe beam beat with the prepared Raman coherence, we found that the prepared Raman coherence replicates the probe beam to its Raman sidebands. The frequency conversion efficiency from the probe beam to the first AS-Raman sideband rises to the maximum (4.7%) at 284 MW/cm 2 , and then falls with the increase of the pumping intensity. This is thought to be due to the fact that some molecules in the first vibrational level incline to go to the higher vibrational level under the higher pumping intensity. For the strong pumping intensity (290 MW/cm 2 ), four anti-Stokes and one Stokes Raman sidebands of the probe beam were generated.
We present a numerical model for the interaction of a femtosecond probe pulse with a Raman medium excited by two nanosecond laser pulses in solid hydrogen. The model consists of a solution of a system of Bloch equations (for the medium state) and of the two-dimensional wave equation (for the field propagation). It is shown that by optimizing the tilt angle between the two driving pulses and the interaction length, the power of the probe pulse can be converted either into a quasicontinuous broadband spectrum or into a selected high-order sideband. The first situation can be used for generation of subfemtosecond pulses. The second situation can be used for the wavelength conversion of a femtosecond probe pulse from the infrared to the ultraviolet region. Due to the transfer of energy from the driving pulses, the energy conversion efficiency of these processes (with respect to the probe pulse) can be larger than unity.