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Applied Optics

Molecular memory effects in transient stimulated Raman scattering in the atmosphere

Bruce J. Herman, Marek J. Konopnicki

Published Jun 15, 1988• 0 citations
Publisher

Abstract

We discuss the enhancement of transient stimulated Raman scattering from a pulse train due to molecular memory effects for atmospheric propagation. For horizontal propagation, we show that enhancement is negligible when the interpulse spacing in the train is >0.1 ns. For propagation up through the atmosphere, the enhancement is a function of interpulse spacing, zenith angle, and pulse energy density.

DOI
10.1364/ao.27.002392

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We discuss the enhancement of transient stimulated Raman scattering from a pulse train due to molecular memory effects for atmospheric propagation. For horizontal propagation, we show that enhancement is negligible when the interpulse spacing in the train is >0.1 ns. For propagation up through the atmosphere, the enhancement is a function of interpulse spacing, zenith angle, and pulse energy density.
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.
Investigations were made of the accumulation effect exhibited by transient electronic stimulated Raman scattering in atomic barium vapor pumped by a train of ultrashort pulses with a controlled time delay between the pulses. The essential feature of the accumulation effect is that the Stokes energy of a pulse is contributed to not only by its own exciting pump pulse, but also by the previous pump pulse, the influence of the latter depending strongly on the ratio of the transverse relaxation time T2 to the interpulse time interval. If one is to observe the accumulation effect in electronic stimulated Raman scattering, it is important to minimize the influence of depletion of the number of atoms. A method based on the accumulation effect for determination of T2 in one laser shot was developed.
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.
We consider transient stimulated Raman amplification of trains of picosecond pulses. In this regime the gain of a single pulse is reduced from its steady-state value because of the inability of the nonlinear polarization to follow the time variations of the pump pulse. In addition oscillatory behavior of the pump and Stokes pulse amplitudes have been predicted in the transient regime in conditions of high pump depletion. When the pump radiation is in the form of a train of pulses whose separation is comparable to or shorter than the dephasing time of the nonlinear medium, increased gain can be experienced by later pulses in the train because they can grow from the material polarization created by earlier pulses. We have analyzed this type of amplification as a function of pulse spacing, pump energy, and pump intensity in the regime of high pump depletion. In addition we have considered the effects of Stark shifts of the two-photon resonant Raman level on the Stokes conversion efficiency. We find that at constant pulse intensity the conversion efficiency increases with time through the pulse train, gradually approaching steady state at low conversion efficiencies at times long compared to T2. The maximum conversion efficiency increases as the pulse spacing is decreased. If the pump depletion is too high the peak conversion of the Stokes oscillates through the train in a manner similar to the oscillations of the intensity of a single pulse. A Stark shift of the resonant level can cause reduced gain as well as introduce phase shifts on the Stokes and pump beams. The effects of these processes on the conversion efficiency are discussed.