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Soviet Journal of Quantum Electronics

Photon echo due to Fermi-resonance vibrational levels of molecules

S V Amel'kin, А. Н. Ораевский

Published Aug 31, 1983• 1 citation
Publisher

Abstract

A nonlinear coherent optical effect is predicted: it is based on compensation of the Doppler phases of Fermi-resonance vibrations of polyatomic molecules in the case of multifrequency laser excitation, resembling the phenomenon of the photon echo in gases. An analysis is made of the formation of radiation at the sum frequency in the case of two-frequency excitation of a combination vibration. It is shown that the new effect can be used for coherent spectroscopy of nonlinear intermode resonances.

DOI
10.1070/qe1983v013n08abeh004578

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A nonlinear coherent optical effect is predicted: it is based on compensation of the Doppler phases of Fermi-resonance vibrations of polyatomic molecules in the case of multifrequency laser excitation, resembling the phenomenon of the photon echo in gases. An analysis is made of the formation of radiation at the sum frequency in the case of two-frequency excitation of a combination vibration. It is shown that the new effect can be used for coherent spectroscopy of nonlinear intermode resonances.
An analytical study of the photon echoes associated with the three-level system interacting resonantly with optical pulses possessing two different frequencies is performed. It is predicted that photon echoes arise at anomalous times corresponding to the correlation between the inhomogeneous broadenings for the different spectral lines as well as at the normal time expected in a simple two-level system. This new effect is caused by the coupling of the two resonant transitions through the common energy level. Furthermore, if the particle does not have inversion symmetry, the echoes with the sum or difference frequency of the exciting optical pulses can be observed in such a system. The quantitative analysis is also given for intensities, direction of propagation and polarizations of the anomalous echoes which depend upon the exciting pulses with different frequency.
This work is devoted to nonlinear effects in the atomic medium excited by multifrequency laser radiation. We have considered collective light scattering in the optically dense medium in conditions of coherent population trapping. Propagation of intermode correlation coefficient was calculated and it was found that correlation can increase in the medium. Light shifts of the coherent population trapping resonances and ways of their suppression were analyzed. Propagation of radiation in the medium with closed excitation scheme was investigated.
Generation of coherent multifrequency optical radiation by means of excitation of mechanical vibration (acoustical oscillation) of a medium along the propagation of resonant laser radiation is proposed. At the same time the vibrating medium becomes transparent for the incident resonant radiation (acoustically induced transparency). We show, that generation of multifrequency radiation takes place in the absence of inversion in two-level quantum system for any energy distribution among the spectral components of the incident (multifrequency in general) field and any amplitude of vibration. Amplitude of vibration determines efficiency of the normal wave generation. Mechanism of the effect is destructive interference of different spectral harmonics of the field components appearing in the frame of vibrating atoms.
A theory of optical echo spectroscopies of large polyatomic molecules in condensed phases is developed. Using phase space correlation functions, we examine the interrelationships among the following optical measurements: ordinary photon echo, stimulated photon echo, accumulated photon echo, incoherent accumulated photon echo, and pump–probe absorption. Conditions for the elimination of inhomogeneous broadening in these experiments are specified. A multimode Brownian oscillator model is used to account for high frequency molecular vibrations, as well as solvent modes, and electronic dephasing processes. The effects of quantum beats, spectral diffusion, and homogeneous dephasing on the echo signals are studied and compared in detail with pump–probe and hole burning spectroscopy.
A review is given of recent theoretical investigations on coherent propagation and nonlinear interaction of multifrequency ultrashort radiation pulses in resonantly absorbing media. An analysis is made of frequency conversion by parametric interaction and stimulated Raman scattering of laser pulses in resonant three-level media. New ways of controlling the parameters of coherent pulses and the use of multifrequency pulses in the spectroscopy of multilevel media are discussed. The experimental capabilities of the investigated effects are considered.