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Soviet Journal of Quantum Electronics

Characteristics of the dynamics of stimulated Raman scattering in a gas excited by a train of short pulses

Nikolai V Kravtsov, Nikolai I Naumkin, V P Protasov

Published Jul 31, 1975• 3 citations
Publisher

Abstract

An investigation was made of the dynamics of stimulated Raman scattering (SRS) in compressed hydrogen excited by a train of short pulses. The observed features of the SRS dynamics were attributed to the competition between the focusing influence of an SRS lens and the defocusing influence of a thermal lens generated as a result of relaxation of an excited state. The method employed made it possible to determine the polarizability of the vibrational state of the molecules excited by SRS.

DOI
10.1070/qe1975v005n07abeh011607

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An investigation was made of the dynamics of stimulated Raman scattering (SRS) in compressed hydrogen excited by a train of short pulses. The observed features of the SRS dynamics were attributed to the competition between the focusing influence of an SRS lens and the defocusing influence of a thermal lens generated as a result of relaxation of an excited state. The method employed made it possible to determine the polarizability of the vibrational state of the molecules excited by SRS.
The high pulse repetition rates (~100 MHz) of radio-frequency free-electron lasers make possible the investigation of molecular response to a rapid pulse train.1 When the molecular decay time T2 is much larger than the time between pulses T, molecular memory is carried from pulse to pulse. For stimulated Raman scattering (SRS) the memory effect can lead to an increase in the size of the Raman dipole resulting in enhanced scattering. We analyze the 1-D SRS equations in the condition that the scattering under an individual pulse occurs in the transient regime (~10 ps). We obtain a general expression for the behavior of SRS which reduces to the following long-time limits: (1) When T2 ≪ T, the SRS from each pulse in the train develops independently from the others; (2) When T2 ≫ T, the transient SRS response is equivalent to the steady-state response to a constant pump at the time-averaged pump intensity. We also perform this analysis for a medium such as the atmosphere where the density of scatterers and Raman bandwidth decrease exponentially with distance.
Summary form only given. We report on the stimulated Raman scattering (SRS) in the liquid hydrogen droplet. Although many works have been carried out so far in terms of the droplet nonlinear optics, this is the first report which investigates the nonlinear optical processes in a droplet that has rotational and vibrational internal freedom. We show that the liquid hydrogen droplet can readily result in a huge cavity Q-value of 10/sup 9/ and that the SRS in the droplet proceeds not only for vibrational transitions but also for vibrational-rotational and pure-rotational transitions as in the gas phase.
An investigation was made of the influence of different excitation conditions on the self-focusing of stimulated Raman-scattered light. It was found that the dimensions of self-focusing filaments and their number depended on the energy of the exciting radiation and the thickness of the scattering layer. In the situation in which self-focusing points were observed at both ends of a Dewar flask, the anti-Stokes scattering included (in addition to rings of class 1) scattering along the axis. Estimates were obtained of the self-focusing threshold power related to the Kerr effect and to the increase in the polarizability of molecules due to excitation. It was found that the first of these mechanisms could not give rise to self-focusing of the Raman-scattered light, whereas the threshold of the second mechanism was close to the excitation energy at which such self-focusing was observed.
The far field direction of propagation of light pulses generated by transient, single pass stimulated Raman scattering (SRS) is observed to fluctuate front pulse to pulse due to quantum mechanical uncertainties in the occupation numbers of different coherent spatial modes. When SRS is generated on the Q(l) vibrational transition in hydrogen with an interaction region Fresnel number near unity, the lowest-order coherent spatial mode dominates the generation process, leading to near-diffraction-limited Stokes light.
An investigation was made of the influence of the geometric excitation conditions on the energy dependences of the stimulated scattering of focused laser pulses of ~ 10 −8 sec duration when the sharpness and depth of focusing were varied. The experimental results obtained in this study were interpreted theoretically on the basis of a quantum analysis of stimulated Raman scattering in a two-level system. The experimental relationships could be explained only if an allowance was made for the changes in the populations of the levels participating in the Raman transition. It was possible to select the experimental conditions so that reconstruction of the wavefront of the pump radiation was observed under stimulated scattering conditions in a wide energy range.