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Internet Electronic Journal of Molecular Design - IEJMD, ISSN 1538-6414, CODEN IEJMAT
ABSTRACT - Internet Electron. J. Mol. Des. April 2004, Volume 3, Number 4, 209-221

Modifications in the Maximal Intensity of Four-Wave Mixing Signal under the Changes of Vibronic Coupling Conditions
José Luis Paz, Teresa Cusati, and Antonio J. Hernández
Internet Electron. J. Mol. Des. 2004, 3, 209-221

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Abstract:
The spectroscopic analysis of the behavior of the nonlinear signal response of systems including electronic levels is described by the coupling parameters of crossed harmonic potential curves. Changes in the Four-Wave Mixing (FWM) signal intensity are originated by the modifications of the dipole moments in the new coupled basis due to variation of the parameters V0 (energetic difference between the minima), v (coupling parameter) and δ (strength constant) corresponding to the crossed states involved. The permanent dipole moments of the states in the uncoupled basis have been included and the Rotating-Wave Approximation is neglected in order to observe the processes out of the resonance region. The calculation method is based in the Liouville-von Neumann formalism for the density matrix, where the Conventional Optical Bloch Equations are solved in the Fourier space to obtain the density matrix elements associated with the Macroscopic Polarization responsible of the FWM signal. Variation in the coupling parameters generates modifications in the dipole moments of the coupled states. These modifications induce changes in the intensity values of the FWM signal, including the nullity of the dipole moments producing the nullity of the nonlinear signal. Mathematical expressions are obtained to interprete these results. Changes in the characteristic coupling parameters induce modifications on the crossed potential curves, and consequently, on the nonlinear response and intensity.

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