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

Résultats de recherche: Contribution dans un livre/un catalogue/un rapport/dans les actes d'une conférenceChapitre (revu par des pairs)

Résumé

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.
langueAnglais
titreFrontiers of Quantum Chemistry
rédacteurs en chefMarek Wojcik, Hiroshi Nakatsuji, Bernard Kirtman, Yokohiro Ozaki
Lieu de publicationSingapore
EditeurSpringer
Pages117-138
Nombre de pages21
ISBN (Electronique)978-981-10-5651-2
ISBN (imprimé)978-981-10-5650-5
Les DOIs
étatPublié - 2018

Empreinte digitale

Optical properties
Molecules
Quantum chemistry
Electron correlations
Solvation
Wave functions
Optoelectronic devices
Photonics
Density functional theory
Experiments

Citer ceci

Champagne, B., Beaujean, P., De Wergifosse, M., Hidalgo Cardenuto, M., Liégeois, V., & Castet, F. (2018). Quantum Chemical Methods for Predicting and Interpreting Second-Order Nonlinear Optical Properties: From Small to Extended π-Conjugated Molecules. Dans M. Wojcik, H. Nakatsuji, B. Kirtman, & Y. Ozaki (eds.), Frontiers of Quantum Chemistry (p. 117-138). Singapore: Springer. https://doi.org/10.1007/978-981-10-5651-2_6
Champagne, Benoît ; Beaujean, Pierre ; De Wergifosse, Marc ; Hidalgo Cardenuto, Marcelo ; Liégeois, Vincent ; Castet, Frédéric. / Quantum Chemical Methods for Predicting and Interpreting Second-Order Nonlinear Optical Properties: From Small to Extended π-Conjugated Molecules. Frontiers of Quantum Chemistry. Editeur / Marek Wojcik ; Hiroshi Nakatsuji ; Bernard Kirtman ; Yokohiro Ozaki. Singapore : Springer, 2018. p. 117-138
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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.",
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Quantum Chemical Methods for Predicting and Interpreting Second-Order Nonlinear Optical Properties: From Small to Extended π-Conjugated Molecules. / Champagne, Benoît; Beaujean, Pierre; De Wergifosse, Marc; Hidalgo Cardenuto, Marcelo; Liégeois, Vincent; Castet, Frédéric.

Frontiers of Quantum Chemistry. Ed. / Marek Wojcik; Hiroshi Nakatsuji; Bernard Kirtman; Yokohiro Ozaki. Singapore : Springer, 2018. p. 117-138.

Résultats de recherche: Contribution dans un livre/un catalogue/un rapport/dans les actes d'une conférenceChapitre (revu par des pairs)

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AU - Liégeois, Vincent

AU - Castet, Frédéric

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N2 - 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.

AB - 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.

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Champagne B, Beaujean P, De Wergifosse M, Hidalgo Cardenuto M, Liégeois V, Castet F. Quantum Chemical Methods for Predicting and Interpreting Second-Order Nonlinear Optical Properties: From Small to Extended π-Conjugated Molecules. Dans Wojcik M, Nakatsuji H, Kirtman B, Ozaki Y, rédacteurs en chef, Frontiers of Quantum Chemistry. Singapore: Springer. 2018. p. 117-138 https://doi.org/10.1007/978-981-10-5651-2_6