Ab initio investigation of the sum-frequency hyperpolarizability of small chiral molecules

Benoît Champagne, Peer Fischer, A. David Buckingham

Research output: Contribution to journalArticle


Using a sum-over-states procedure based on configuration interaction singles /6-311++G**, we have computed the sum-frequency hyperpolarizability βijk(-3ω;2ω,ω) of two small chiral molecules, R-monofluoro-oxirane and R-(+)-propylene oxide. Excitation energies were scaled to fit experimental UV-absorption data and checked with ab initio values from time-dependent density functional theory. The isotropic part of the computed hyperpolarizabilities, β̄(-3ω;2ω,ω), is much smaller than that reported previously from sum-frequency generation experiments on aqueous solutions of arabinose. Comparison is made with a single-centre chiral model.

Original languageEnglish
Pages (from-to)83-88
Number of pages6
JournalChemical Physics Letters
Issue number1
Publication statusPublished - 24 Nov 2000


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