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NANOSYSTEMS: PHYSICS, CHEMISTRY, MATHEMATICS, 2012, 3 (2), P. 55–64

NONLINEAR OPTICAL CHANNELS OF POLARIZABILITY INDUCTION IN A PAIR OF INTERACTING MOLECULES

A.P. Kouzov – Saint-Petersburg State University, Saint-Petersburg, Russia; Doctor of Physics and Mathematics, Leading Researcher; alex@ak1197.spb.edu
N.I. Egorova – Saint-Petersburg State University, Saint-Petersburg, Russia; Candidate of Physics and Mathematics; Assistant.
M. Chrysos – Université d’Angers, Angers, France; Docteur de Sciences, Professeur.
F. Rachet – Université d’Angers, Angers, France; Docteur de Sciences, Maître de Conférences.

Intermolecular interactions induce additional terms of polarizability of a molecular ensemble and thus allow the vibrational Raman transitions forbidden by the selection rules for isolate molecules. Based on the diagrammatic technique, a new long-range induction channel of the binary polarizability is established for which the outer field and the electric field of one
molecule nonlinearly polarize the partner particle. An account for this channel is demonstrated to be crucial for an exhaustive quantitative interpretation of the CO2 ν3 Raman band induced by the CO2-CO2 and CO2-Ar collisions.
Keywords: spectroscopy of intermolecular interactions, Raman scattering, nonlinear polarization of molecules.

UDC 535.375.5, 539.6

PACS 31.15.-p, 33.20.Ea, 33.20.Fb, 33.15.Kr, 33.15.-e, 34.20.-b, 95.30.Ky

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