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Journal of Molecular Spectroscopy

Study and Characterization of Resonances in the Four-Wave Mixing Signal of a Two-Level System with Intramolecular Coupling

José Luis Paz, Teresa Cusati, M. C. Salazar, A. J. Hernández

Published Feb 1, 2002• 6 citations
Publisher
DOI
10.1006/jmsp.2001.8499

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We consider the Four-Wave mixing (FWM) signal and the effects of the pump beam on the nonlinear optical responses of a two-level system where intramolecular coupling is modelled by two coupled harmonic electronic potentials, displaced both in their equilibrium minimum position and energy. We investigate the modifications introduced in the FWM signal, considering a simple representation for the vibrational structure and including molecular electronic states with nonzero permanent dipole moments. The critical quantities for this analysis are the transition and permanent dipole moments, which depend strongly on the intramolecular coupling. Our results show how both absorption and dispersion are affected by the vibronic coupling.
A study has been made of the effect of relaxation times on the four-wave mixing (FWM) signal response in frequency space for a two-level system where intramolecular coupling is explicitly taken into account within a vibronic model. The model is a generalization of the conventional two-level approach in that it includes a simplified description of the molecular structure and the explicit consideration of permanent dipole moments. Significant changes in both the intensity and shape of the peaks of the FWM spectrum are observed, due mainly to changes in the ratio between the longitudinal and transversal relaxation times, T 1/T 2.