Solvent influence on the nonlinear optical properties of molecular systems in the presence of degenerate and non-degenerate four-wave mixing

The nonlinear optical properties are studied theoretically of a molecular system immersed in a thermal bath and interacting with a four-wave mixing signal. A methodology based on cumulant expansions to obtain the average in the Fourier components associated with the coherences and populations, calcu...

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Bibliographic Details
Published in:Journal of modern optics 2012-01, Vol.59 (1), p.71-82
Main Authors: Paz, J.L., Mendoza-García, A.
Format: Article
Language:English
Subjects:
Beams (radiation)
Electric noise
Four-wave mixing
Frequencies
Mathematical models
nonlinear optical properties
Nonlinearity
Optical properties
optical stochastic Bloch equation
Populations
Pulsation
Relaxation time
Solvents
white noise
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Summary:The nonlinear optical properties are studied theoretically of a molecular system immersed in a thermal bath and interacting with a four-wave mixing signal. A methodology based on cumulant expansions to obtain the average in the Fourier components associated with the coherences and populations, calculated by the optical stochastic Bloch equations, is employed. The system properties are analyzed as a function of the frequency detuning of the high-intensity pump beam and parameterized by the frequency detuning of the probe beam, both with respect to the Bohr frequency of the system. The longitudinal and transversal relaxation times and the bath effects, modeled as white noise, are also included as parameters in the calculation. Different cases, with degenerate and non-degenerate optical frequencies are examined and compared, resulting in differences related to the maximum in the population pulsation effects.
ISSN:0950-0340
1362-3044
DOI:10.1080/09500340.2011.639962