Nonlinear optical responses of molecular systems with vibronic coupling in fluctuating environments

Author:

Paz Jose Luis1,Loroño Marcos2,González-Paz Lenin A.3,Marquez Edgar4,Vera-Villalobos Joan5,Mora José R.6,Alvarado Ysaias J.7

Affiliation:

1. Departamento Académico de Química Inorgánica, Facultad de Química e Ingeniería Química, Universidad Nacional Mayor de San Marcos, Lima, Perú

2. Departamento Académico de Química Analítica e Instrumental, Facultad de Química e Ingeniería Química, Universidad Nacional Mayor de San Marcos, Lima, Perú

3. Laboratorio de Genética y Biología Molecular (L.G.B.M), Departamento de Biología Facultad Experimental de Ciencias (F.E.C), Universidad del Zulia (LUZ) Maracaibo, República Bolivariana de Venezuela

4. Grupo de Investigaciones en Química y Biología, Departamento de Química y Biología, Facultad de Ciencias Exactas, Universidad del Norte, Carrera 51B Km 5, Vía Puerto Colombia, Barranquilla 081007, Colombia

5. Escuela Superior Politécnica del Litoral, Facultad de Ciencias Naturales y Matemáticas, Ecuador

6. Universidad San Francisco de Quito, Grupo de Química Computacional y Teórica (QCT-USFQ), Departamento de Ingeniería Química, Diego de Robles y Vía Interoceánica, Quito, 170901, Ecuador

7. Laboratorio de Caracterización Molecular y Biomolecular, Centro de Investigación y Tecnología de Materiales (CITeMA), Instituto Venezolano de Investigaciones Científicas (IVIC), Maracaibo, Estado Zulia República Bolivariana de Venezuela

Abstract

The topological profiles of the nonlinear optical properties of a two-level molecular system involving simplified versions of intramolecular coupling immersed in a thermal reservoir have been studied in four-wave mixing (FWM) spectroscopy. Solvent effects have been explicitly considered by modeling the nonradiative interaction with the solute as a random variable. To formulate a solution, it is necessary to introduce stochastic considerations. We assume that system–solvent interactions induce random shifts in the Bohr frequency of the adiabatic states, and their manifestation corresponds to the broadening of the upper level. The Born–Oppenheimer (BO) electronic energy curves for this molecular model consist of two intertwined harmonic oscillator potentials shifted in both their position and their minimum equilibrium energy. The critical quantities for this analysis are the transition and permanent dipole moments, which depend strongly on intramolecular coupling. Our results show how absorption and refractive index are affected by vibronic coupling and solvent stochasticity.

Publisher

World Scientific Pub Co Pte Ltd

Subject

Physics and Astronomy (miscellaneous),Atomic and Molecular Physics, and Optics,Electronic, Optical and Magnetic Materials

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