Lomakin G.S., Ivanov A.I., Мikhailova V. A. Calculation of the spectral dynamics of systems with a quadratic vibronic interaction

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Lomakin Gennady Sergeevich

PhD, senior researcher at the Laboratory of Theoretical Physics Institute of Physics of Molecules and Crystals, Ufa Scientific Center, Russian Academy of Sciences
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Prospect Oktyabrya, 71, 450075, Ufa, Russian Federation

Ivanov Anatoly Ivanovich

Doctor of Sciences, Professor of Department of Theoretical Physics and Wave Processes, Physical-Technical Institute, Volgograd State University
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Prospect Universitetsky, 100, 400062 Volgograd, Russian Federation

Мikhailova Valentina Alexandrovna

Doctor of Sciences, Professor of Department of Theoretical Physics and Wave Processes, Physical-Technical Institute, Volgograd State University
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Prospect Universitetsky, 100, 400062 Volgograd, Russian Federation

Abstract. Progress in generating ultrashort laser pulses provides continuous development of the exploration methods of the transient emission and absorption spectra. The theoretical approaches are basically limited to linear electron-vibrational interaction. In this paper the influence of quadratic vibronic interaction on transient spectra is explored. The method of functional derivatives is applied for calculation of the generating function determining the optical spectrum of a two-level electron-vibration system. The analytical expression for the generating function for the two-level electron-vibration system with quadratic vibronic interaction is derived. It is found that the frequency change of the vibrational subsystem accompanying the electronic transition manifests itself in both the first and second cumulants of the optical spectrum. The second cumulant defines the frequency dispersion is not the same for stationary and non-stationary spectra. The evolution equation of the second cumulant is obtained. An analytical expression for the first cumulant determining the position of the spectrum gravity center is derived. The time dependent displacement of the spectrum gravity center is demonstrated to be accompanied by a change in its width. It is shown that in the absence of the frequency change of the vibrational subsystem the generating function is transformed to a form received earlier at the description of ultrafast dynamics of the reverse transition from a state produced by a short laser excitation of a donor-acceptor complex at the frequency of the charge transfer absorption band.

Key words: hot spectroscopy, optical spectra, generating function, vibrational relaxation, spectral dynamics.

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Calculation of the spectral dynamics of systems with a quadratic vibronic interaction by Lomakin G.S., Ivanov A.I., Мikhailova V. A. is licensed under a Creative Commons Attribution 4.0 International License.

Citation in English: Science Journal of Volgograd State University. Mathematics. Physics. №2 (19) 2013 pp. 85-98

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