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Journal of the Optical Society of America B

Stimulated Raman scattering in the transient limit

Godehard Hilfer, Curtis R. Menyuk

Published May 1, 1990• 44 citations
Publisher

Abstract

Stimulated Raman scattering is considered in the transient limit where the pulse width is small compared with T2. In the case where diffraction, level saturation, anti-Stokes and higher-order Stokes radiation, and quantum noise can all be neglected, we show that there are three distinct evolution regimes: the I regime, where the Stokes pulse is small compared with the pump pulse; the transition regime, where the Stokes and pump pulses are comparable; and the J regime, where the pump pulse is small compared with the Stokes pulse. The characteristic behavior in each of these three regimes is explored by using a combination of analytical and numerical tools.

DOI
10.1364/josab.7.000739

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Stimulated Raman scattering is considered in the transient limit where the pulse width is small compared with T2. In the case where diffraction, level saturation, anti-Stokes and higher-order Stokes radiation, and quantum noise can all be neglected, we show that there are three distinct evolution regimes: the I regime, where the Stokes pulse is small compared with the pump pulse; the transition regime, where the Stokes and pump pulses are comparable; and the J regime, where the pump pulse is small compared with the Stokes pulse. The characteristic behavior in each of these three regimes is explored by using a combination of analytical and numerical tools.
Manifestations of quantum fluctuations in stimulated Raman scattering ( SRS ) have been intensively studied lately1. Quantum noise present in spontaneous scattering stimulates fluctuations both in phase and in amplitude characteristics of output Stokes emission. At present statistical properties of amplitude fluctuations are studied in detail and it is shown that in linear transient regime of SRS without pump depletion statistical scatter of Stokes energy Es has negative exponential distribution2. In saturation regime of SRS the amplitude fluctuations are almost suppressed simultaneously with pump depletion. The phase fluctuations manifest both in linear and in nonlinear SRS and produce beam pointing fluctuations3, a change in Stokes emission spectra from pulse to pulse4 and cause soliton appearance in Rayleigh component of SRS5. Phase noise is observed in saturation regime due to relation between phases of Stokes and phonon waves which is preserved in processes of stationary and quasistationary SRS amplification. Spectrum phase fluctuations manifest as fine structure of SRS spectrum4, fluctuations of average Stokes frequency and Stokes linewidth fluctuations. The evolution of phase fluctuations in time is determined by the nature of spontaneous scattering and polarization of Raman media and is of great interest as one can follow its development from vacuum modes level to saturation regime. However up to now this problem has not been studied yet.
In transient stimulated Raman scattering (SRS), efficient conversion of short pump pulses to Stokes radiation is difficult to obtain. A short seed pulse at the Stokes frequency increases the efficiency and may induce full depletion of the pump pulse, even when the pump power is too low to scatter efficiency without seed. However, for low pump powers the Ra­man polarizability induced by the pump and seed pulse decays, which results in a terminating Stokes pulse, even when the pump pulse itself is long. Nevertheless, the Stokes pulse can be wider than the dephasing time of the Raman polarizability or the width of the seed pulse by an order of magnitude. Applying a second seed may once again induce a sufficiently large Raman polarizability but only if the phase of the Stokes seed matches the phase difference between the pump and remaining Raman polarizability. If not, the polarizability induced by the first pulse and consequently the conversion efficiency for the Stokes radiation decreases. Therefore, it is possible to switch off the Stokes pulse by applying a second seed with appropriate phase and intensity.
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.
Parametric instability induced by the medium saturation in stimulated Raman scattering is investigated theoretically via a generalized detuning (1) where ω p,s,o are the frequency of the pump, Stokes, and phonon, ϕ ˙ p s is the phase modulation, and the last term is the nonlinear correction of the highly excited anharmonic molecule with an amplitude Q.The steady-state gain and hence the Stokes efficiency, in the presence of the anharmonic term, are governed by a cubic equation of |Q|2which is to be solved from the Bloch and Maxwell equations including the pump depletion. Numerical results are shown for the transition diagram of Stokes efficiency vs input pump intensity at various system conditions at the steady-state. For the transient regime, with pulse duration shorter than the dephasing time, we analyze the temporal profiles of the Stokes and the depleted pump based on a transformed equation which combines Bloch and Maxwell equation as follows: (2) where Tis a nonlinear time, G s is the steady-state gain, l0is the input pump intensity, and Uis the real part of the phonon amplitude Q.For an input pulse intensity given by sech2(t/t p ), Eq. (2) is solved numerically to study the transient pulse profiles in the presence of pump depletion and medium saturation.