Title

General model for the description of the third-order optical nonlinearities in conjugated systems: Application to the all-trans beta-carotene molecule

Authors

Authors

D. Beljonne; J. Cornil; Z. Shuai; J. L. Bredas; F. Rohlfing; D. D. C. Bradley; W. E. Torruellas; V. Ricci;G. I. Stegeman

Comments

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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

WOS:A1997YB13900012

ISSN

0163-1829

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