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 Β-carotene molecule by means of the sum-over-states 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.
Original language | English (US) |
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Pages (from-to) | 1505-1516 |
Number of pages | 12 |
Journal | Physical Review B - Condensed Matter and Materials Physics |
Volume | 55 |
Issue number | 3 |
DOIs | |
State | Published - 1997 |
Externally published | Yes |
Bibliographical note
Generated from Scopus record by KAUST IRTS on 2019-11-27ASJC Scopus subject areas
- Electronic, Optical and Magnetic Materials
- Condensed Matter Physics