Title
General model for the description of the third-order optical nonlinearities in conjugated systems: Application to the all-trans beta-carotene molecule
Abbreviated Journal Title
Phys. Rev. B
Keywords
NITRO-STILBENE DANS; 3RD-HARMONIC GENERATION; 2-PHOTON ABSORPTION; ELECTRONIC EXCITATIONS; 2ND HYPERPOLARIZABILITY; INTERCHAIN DISPERSION; RELAXATION ENERGIES; RAMAN EXCITATION; POLYMERS; POLYENES; Physics, Condensed Matter
Abstract
On the basis of an extended configuration-interaction description of the lowest singlet excited states, we investigate the third-order nonlinear optical response of the beta-carotene molecule by means of the sum-overstates approach. We first uncover the nature of the electronic states contributing primarily to the cubic molecular polarizabilities. From this starting point, we apply a simplified model to evaluate the frequency-dependent third-harmonic generation (THG) and electroabsorption (EA) spectra; the vibronic structure of the spectra is described by taking into account Franck-Condon factors calculated in a displaced oscillator model. For both the THG and EA processes, we obtain good agreement between the theoretical simulations and the experimental data, which underlines the general character of our model.
Journal Title
Physical Review B
Volume
55
Issue/Number
3
Publication Date
1-1-1997
Document Type
Article
Language
English
First Page
1505
Last Page
1516
WOS Identifier
ISSN
0163-1829
Recommended Citation
"General model for the description of the third-order optical nonlinearities in conjugated systems: Application to the all-trans beta-carotene molecule" (1997). Faculty Bibliography 1990s. 1843.
https://stars.library.ucf.edu/facultybib1990/1843
Comments
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