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

    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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