Investigation of the linear and second-order nonlinear optical properties of molecular crystals within the local field theory

Tomasz Seidler, Katarzyna Stadnicka, BenoÎt Champagne

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Abstract

In this paper it is shown that modest calculations combining first principles evaluations of the molecular properties with electrostatic interaction schemes to account for the crystal environment effects are reliable for predicting and interpreting the experimentally measured electric linear and secondorder nonlinear optical susceptibilities of molecular crystals within the experimental error bars. This is illustrated by considering two molecular crystals, namely: 2-methyl-4-nitroaniline and 4-(N,Ndimethylamino)- 3-acetamidonitrobenzene. Three types of surrounding effects should be accounted for (i) the polarization due to the surrounding molecules, described here by static electric fields originating from their electric dipoles or charge distributions, (ii) the intermolecular interactions, which affect the geometry and particularly the molecular conformation, and (iii) the screening of the external electric field by the constitutive molecules. This study further highlights the role of electron correlation on the linear and nonlinear responses of molecular crystals and the challenge of describing frequency dispersion.

Original languageEnglish
Article number114105
JournalThe journal of chemical physics
Volume139
Issue number114105
DOIs
Publication statusPublished - 2013

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Molecular crystals
Optical properties
optical properties
Electric fields
crystals
Electron correlations
Molecules
Charge distribution
environment effects
Coulomb interactions
electric fields
Conformations
molecular properties
Screening
Polarization
charge distribution
electric dipoles
molecules
Crystals
screening

Cite this

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