Nonlinear optical properties in molecular systems with non-zero permanent dipole moments in four-wave mixing under stochastic considerations
The solvent effects over nonlinear optical properties of a two-level molecular system in presence of a classical electromagnetic field were modeled in this work. The collective effects proper of the thermal reservoir are modeled as a random Bohr frequency, whose manifestation is the broadening of th...
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| Formato: | Libros |
| Lenguaje: | eng |
| Publicado: |
2017
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| Materias: | |
| Acceso en línea: | http://repositorio.educacionsuperior.gob.ec/handle/28000/5084 |
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| Sumario: | The solvent effects over nonlinear optical properties of a two-level molecular system in presence of a classical electromagnetic field were modeled in this work. The collective effects proper of the thermal reservoir are modeled as a random Bohr frequency, whose manifestation is the broadening of the upper level according to a prescribed random function. A technique of work, based in the use of the cumulant expansions to obtain the average in the Fourier components associated with the coherence and populations, evaluated by the use of the Optical Stochastic Bloch Equations (OSBE), is employed. Analytical expressions for susceptibility, optical properties and non-degenerate Four-Wave Mixing (nd-FWM) signal intensity, were obtained. Numerical calculations were carried out to construct surfaces corresponding to these magnitudes as a function of the pump-probe frequency detuning, values of the permanent dipole moments (PDM), noise parameters and relationships between the longitudinal and transversal relaxation times. Our results show that it is necessary to neglect the Rotating-Wave approximation (RWA) in order to measure the effect of the permanent dipole moments and that the inclusion of these favors two-photon transitions over those with one-photon. In general, the effect of non-zero permanent dipole moments, are reflected in the appearance of new and more complex signals associated with new multiphoton processes. |
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