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Quantum Electronics

Raman response of polar molecules to quasiresonant radiation

Valery S. Butylkin

Published Sep 30, 1994• 0 citations
Publisher

Abstract

A theoretical investigation is reported of the Raman scattering in the rf range by polar molecules. It is shown that an increase in the Stokes frequency ω s (from zero) results in an increase in the imaginary part of the susceptibility, which governs the spontaneous Raman scattering cross section and the stimulated Raman scattering increment. This increase in the susceptibility is faster than in the optical range by a factor of ω s 2 . The susceptibility maximum occurs at the Stokes frequency and its width is of the order of the width of the transition line at which the Raman scattering takes place. A further increase in the frequency reduces the resonant contribution to the Raman scattering, and the frequency dependences of the parameters of this contribution approach the dependences typical of the optical range. The influence of the saturation effects on the resonant Raman response is pointed out.

DOI
10.1070/qe1994v024n09abeh000247

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•Jan 1, 1978•0 citations
A theoretical investigation is reported of the Raman scattering in the rf range by polar molecules. It is shown that an increase in the Stokes frequency ω s (from zero) results in an increase in the imaginary part of the susceptibility, which governs the spontaneous Raman scattering cross section and the stimulated Raman scattering increment. This increase in the susceptibility is faster than in the optical range by a factor of ω s 2 . The susceptibility maximum occurs at the Stokes frequency and its width is of the order of the width of the transition line at which the Raman scattering takes place. A further increase in the frequency reduces the resonant contribution to the Raman scattering, and the frequency dependences of the parameters of this contribution approach the dependences typical of the optical range. The influence of the saturation effects on the resonant Raman response is pointed out.
The temperature effect on the resonance Raman scattering from molecules is investigated. Considering a total system consisting of a molecular system, a heat bath, and the weak radiation field, a general expression for the relaxation processes is derived utilizing the Liouville operator technique for the time evolution of the density matrix of the total system. By using the perturbation method with respect to the radiation and matter up to second order, rate constants for zero photon (radiationless processes), one-photon and two-photon processes are derived after taking the long time limit in the Markoff approximation. Assuming a weak interaction between the molecular system and heat bath, a temperature-dependent resonance Raman scattering cross section is formulated in the adiabatic basis set for the molecular systems. In the displaced harmonic oscillator model, we obtain an analytical expression for the temperature-dependent Raman scattering cross section for the multimode case, which is suitable for both weak coupling and strong coupling cases. Analytical expressions for the Stokes and anti-Stokes bands of the jth order vibrational transition in the one oscillator model can easily be obtained from the general expression for the resonance Raman scattering cross section derived. An approximate Stokes to anti-Stokes ratio is given up to the second order of the dimensionless displacement Δ. The resonance Raman scattering cross section and the excitation energy profiles are numerically calculated as a function of physical constant such as temperature, molecular vibrational frequency and Δ. It is shown that the excitation profiles of the anti-Stokes band of the jth order vibrational transition have the similar envelope of the corresponding Stokes band shifted by jh/ω. The inverse Raman effect which is closely related to the ordinary Raman effect is also discussed.
A simple description of the stimulated Raman emission of Stokes radiation, and of the induced absorption found by Stoicheff at the anti-Stokes frequency, is based on the semiclassical theory of radiation. This theory gives the well-known formulas for absorption and stimulated emission when carried to the first order in the time-dependent perturbation due to the interaction of the light beam with the molecules. If there are two light beams of frequencies ωL and ω, the second-order perturbation may be associated with stimulated emission at the Stokes frequency ω=ω−1=ωL—ωR and with induced absorption at the anti-Stokes frequency ω=ω1=ωL+ωR, where ωL is the laser frequency and ωR a Raman-active vibrational frequency; in both cases, there is a molecular transition to the excited vibrational state. The highly directional and very sharp anti-Stokes emission at ω1 arises from the conversion by molecules in intense beams at ωL and ω−1 of two ωL photons into an ω−1, ω1 pair. Like spontaneous emission from excited states, the production of this anti-Stokes radiation requires the full quantum theory of radiation for an adequate description. The emission of ω1 and the observed directional absorption of ω−1 due to the reverse conversion ω−1+ω1→2ωL are explained. The anti-Stokes emission is proportional to the Stokes intensity and to the square of that of the laser, and to the square of the molecular number density; its sharpness is due to the absence of a molecular transition. The generation of photon pairs ω−n+ωn, where ωn=ωL+nωR, can occur for all values of n, but it is most efficient for n=1, due to resonance in the appropriate molecular hyperpolarizability and to the intensity of the Stokes beam at ω−1.
The influence of a strong field resonant to the Raman transition on the behavior of the Stokes harmonic in saturated two-wave stimulated Raman scattering is theoretically considered based on the description of a gas of three-level atoms by medium density matrix equations. The vibrational mode of energy redistribution between laser and scattered radiation, threshold with respect to the resonant field intensity, is predicted. The action of optical fields on the absorption and amplification of the resonant field in a Raman medium is described.
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 stimulated Raman scattering (SRS), arising from the interaction between molecules of a medium and two strong light fields - a resonant field and a pumping field - is studied theoretically. The transitions of molecules between a given pair of levels is assumed to be both Raman active and infrared active. A semiclassical approach, in which the density matrix method is used for the quantum mechanical description for the medium, is employed. We expand the density matrix in various orders within which the zeroth-order is referred to as the solution of the equation of motion of the density matrix when only the resonant field is applied. -- We obtain a set of equations in second order of the density matrix element p₁₀⑵ (ω) from which the gain function can be derived. This set of equations in the special case of steady state is accidentally similar to those obtained by Mollow in his study of the power spectrum of a strong driven two-level system. We have shown that the SRS in the steady state under the resonant field interaction, is drastically reduced in general. When the flopping frequency is larger than the relaxation constants (Ω > r), we find there appears both weak positive and weak negative gains on both sides of the ordinary SRS components. Since we retain our second-order equations in a general form rather than the form for steady state, we are able to take account of the dependence on the transient zeroth solution. By employing the Laplace transform technique with the help of convolution products, we are able to solve for ρ₁₀⑵(ω) in the stationary flopping state. When the intensity of the resonant field is high, we have found theoretically that both the Stokes and anti-Stokes component become doublets and equally displaced by the amount of the flopping frequency, Ω, on the opposite sides of ordinary Stokes and anti-Stokes components, respectively. The gain maxima are approximately the order of Ω/4r times the ordinary gain of the Stokes component, where Ω/r >> 1 if the flopping exists. The gains are therefore large in comparison with the ordinary gain for SRS in the steady state.