First-principles determinations and investigations of the electronic absorption and third-order polarizability spectra of electron donor-acceptor chromophores tetraalkylammonium halide/carbon tetrabromide

Juan Shen, Wen Dan Cheng, Dong Sheng Wu, Shuping Huang, I. Hu, Zhi Xie

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4 Scopus citations

Abstract

Calculations on donor-acceptor molecular pairs of tetraalkylammonium halide/carbon tetrabromide complexes are provided to investigate structure/property-related linear and nonlinear optical properties by using the time-dependent density functional theory technique coupled with the sum-over-states method. The calculated energies of the first allowed electronic transition decrease, and the nonresonant third-order polarizabilities at the THG, EFISHG, and DFWM optical processes increase progressively from [DBU-H +Br-·CBr4] to [NPr4Br· CBr4] to [NMe4Br·CBr4]. The obtained electronic absorption spectra show a progressive red shift with increasing donor strength from Cl to I for [NR4h·CBr4] (h = Cl, Br, and I). The charge transfers from the halogen donor to the carbon tetrabromide acceptor make significant contributions to the electronic absorption spectra in the low-energy zone and the third-order polarizabilities in the nonresonant frequency region. The counterion indirectly affects the electronic absorption and third-order polarizability spectra through the interactions between the donor and acceptor.

Original languageEnglish (US)
Pages (from-to)9249-9254
Number of pages6
JournalJournal of Physical Chemistry A
Volume111
Issue number38
DOIs
StatePublished - Sep 27 2007

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