Theoretical study of two-photon absorption in donor-acceptor chromophores tetraalkylammonium halide/carbon tetrabromide

Juan Shen, Wen Dan Cheng, Dong Sheng Wu, You Zhao Lan, Fei Fei Li, Shuping Huang, Hao Zhang, Ya Jing Gong

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Two-photon absorption properties of a series of donor-acceptor chromophores of tetraalkylammonium halide/ carbon tetrabromide ([NR4h· CBr4], h = Cl, Br, I; R = Me, Et, Pr) complexes are investigated in terms of the calculated results by the time-dependent density functional theory (TDDFT) technique combined with the sum-over-states (SOS) method. The modeling two-photon absorption spectra show that these charge-transfer complexes have large two-photon absorption (TPA) cross sections and the [NEt 4I·CBr4] has the largest TPA cross section δ with the value of 5.0 × 10-45 cm4 s photon -1. The maximum values of δ increase with increasing separations between the donor/acceptor in the order Cl⋯Br < Br⋯-Br < I⋯Br for [NEt4h·CBr4] complexes; however, the TPA cross sections δ vary slightly as the size of the alkyl group increases from methyl to propyl for the bromide as a donor, and the maximum wavelength of the TPA peak λmax indicates a bathochromic shift. The charge transfers from the halide anion to the carbon tetrabromide make a significant contribution to the excited states, and the donor-acceptor charge transfer plays an important role in the TPA activity, whereas changes in size of alkyl group do not make a substantial contribution to TPA.

Original languageEnglish (US)
Pages (from-to)10330-10335
Number of pages6
JournalJournal of Physical Chemistry A
Issue number34
StatePublished - Aug 31 2006


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