Quantum-chemistry simulations of second-harmonic and sum-frequency generation of organic layers

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By using quantum-chemistry approaches, the second-order nonlinear optical responses of molecules and two-dimensional molecular arrays containing the p-nitroaniline chromophore are evaluated in order to highlight key features of the simulation of the second-harmonic and sum-frequency generation spectra of organic layers. For the electronic component, which dominates the second-harmonic generation response and which constitutes the weakly frequency-dependent background contribution to the vibrational sum-frequency generation phenomenon, the time-dependent Hartree-Fock scheme based on the semi-empirical AM1 parameterization is suitable for predicting the microscopic responses as well as for accounting for the surrounding effects within a simple multiplicative scheme. For the vibrational resonant part of the sum-frequency generation response, ab initio density functional theory approaches turn out to be necessary for locating the resonances and estimating their intensities.

Original languageEnglish
Pages (from-to)627-634
Number of pages8
JournalApplied physics. B: Lasers and optics
Issue number7-8
Publication statusPublished - 1 May 2002

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