Quantum Chemical Methods for Predicting and Interpreting Second-Order Nonlinear Optical Properties: From Small to Extended π-Conjugated Molecules

Benoît Champagne, Pierre Beaujean, Marc De Wergifosse, Marcelo Hidalgo Cardenuto, Vincent Liégeois, Frédéric Castet

Research output: Contribution in Book/Catalog/Report/Conference proceedingChapter (peer-reviewed)

Abstract

This chapter addresses the methodological and computational aspects related to the prediction of molecular second-order nonlinear optical properties, i.e., the first hyperpolarizability (β), by using quantum chemistry methods. Both small (reference) molecules and extended push-pull π-conjugated systems are considered, highlighting contrasted effects about (i) the choice of a reliable basis set together with the convergence of β values as a function of the basis set size, (ii) the amplitude of electron correlation contributions and its estimate using wave function and density functional theory methods, (iii) the description of solvent effects using implicit and explicit solvation models, (iv) frequency dispersion effects in off-resonance conditions, and (v) numerical accuracy issues. When possible, comparisons with experiment are made. All in all, these results demonstrate that the calculations of β remain a challenge and that many issues need to be carefully addressed, pointing out difficulties toward elaborating black-box and computationally cheap protocols. Still, several strategies can be designed in order to achieve a targeted accuracy, either for reference molecules displaying small β responses or for molecules presenting large β values and a potential in optoelectronics and photonics.
Original languageEnglish
Title of host publicationFrontiers of Quantum Chemistry
EditorsMarek Wojcik, Hiroshi Nakatsuji, Bernard Kirtman, Yokohiro Ozaki
Place of PublicationSingapore
PublisherSpringer
Pages117-138
Number of pages21
ISBN (Electronic)978-981-10-5651-2
ISBN (Print)978-981-10-5650-5
DOIs
Publication statusPublished - 2018

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    CHAMPAGNE, B., Lazzaroni, R., Geuzaine , C., Chatelain, P. & Knaepen, B.

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