Autler-Townes splitting of photoelectron energy distributions in resonant twophoton ionisation is predicted using standard Heitler-Ma techniques.
One of the significant problems of molecular spectroscopy is the determination and detailed analysis of how molecular vibrations are dephased. The dephasing of infrared-active (IR-active) vibrations of molecules was investigated by IR absorption spectroscopy. Pulse methods were used to investigate IR-vibrations as well. These methods revealed such coherent nonstationary effects as optical nutation, damping of the free polarization, photon echo, etc. New means of studying dephasing processes were uncovered by the method of nonstationary (time-domain) coherent anti-Stokes Raman scattering (CARS) spectroscopy. However, there are some aspects of CARS that still are not fully covered. One of them is related to Raman scattering by polaritons in dipole-active crystals whereas the second one is the increase of efficiency of CARS (minimization of the wave mismatch, the relationship between pulse width and the relaxation time, etc.). The purpose of the present research to study the case of "extreme" coherency between all interacting pulses (the duration of each pulse is smaller than characteristic times and those pulses are traveling with the same speed) in dipole-active crystals. In this research, we analyzed the process of simultaneous propagation of three waves (anti-Stokes, Stokes, and the pump) under CARS by polaritons. We have found some solutions modeling such simultaneous propagation. We also found the expression for the gain factor for such scattering. The gain factor was evaluated under the assumption of a given stationary pump field. It was shown that the typical values of the relative intensities were consistent with the experimental results.
The system of nonlinear equations modeling the process of nonstationary stimulated Raman scattering (SRS) in noncentrosymmetric crystals for the waves on laser, Stokes, polariton, and phonon frequencies is investigated by using the numerical methods. The general case for amplitudes of waves that resulted in doubling of the number of equations is considered. It is shown that the application of the methods of finite differences to the computer simulation of transition regimes is completely consistent with the analytical results found for the asymptotical solutions in form of solitons. The obtained results also indicate that the laser pulses of Gaussian shape appearing at the boundary of nonlinear medium tend to become solitons of Lorentzian shape. It was also found that the formation of solitons occurs when the vibrations of optical phonons and that of electromagnetic wave were either in or out of phase. It is shown that all electromagnetic waves entering the medium with different speeds become solitons having the same speed. In the second part of the paper we considered the computer simulation of soliton stability with respect to small (weak) perturbations of all interacting waves. In the present paper we considered the case of evolution of those disturbances in the vicinity of peaks of solitons. The numerical analysis showed that in wide range of parameters the solitons were stable.
The purpose of this article is to consider two aspects of the nonstationary stimulated Raman scattering by polaritons in cubic crystals. The first feature is related to the pump field, which, by deforming the permittivity of the medium, changes its symmetry. As a result, for example, the cubic crystal becomes anisotropic. The second one results from the possibility of exciting anomalous longitudinal waves at the frequency of the mechanical phonons which is the fundamental difference between scattering by dipole-active (polar) phonons and that of by dipole-inactive (nonpolar) ones. When the phonon frequency is approached, the amplitude of the transverse polariton wave decreases due to increased absorption and the wave mismatch. The polariton wave becomes practically longitudinal. Such a wave is maintained by the pump field and exists only in a pumped medium. The system of four shortened nonstationary equations (two for the Stokes waves with perpendicular polarizations and two for both transverse and longitudinal polariton waves) is obtained. The analysis is carried out for a given stationary pump field which is assumed to be a linearly polarized plane electromagnetic wave. Principal attention was paid to the calculation and analysis of the gain factor which defines the intensities of both stimulated (SRS) and spontaneous Raman scattering. The expressions for two proper gain factors g µ are obtained for Stokes waves in nonstationary case. It was shown that the pumped cubic crystal becomes anisotropic. It is also shown that the values of intensities calculated by using the expression for g µ are consistent with the experimental results for spectra of ZnS.
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