Abstract
| Original language | English |
|---|---|
| Title of host publication | Frontiers of Quantum Chemistry |
| Editors | Marek Wojcik, Hiroshi Nakatsuji, Bernard Kirtman, Yokohiro Ozaki |
| Place of Publication | Singapore |
| Publisher | Springer |
| Pages | 117-138 |
| Number of pages | 21 |
| ISBN (Electronic) | 978-981-10-5651-2 |
| ISBN (Print) | 978-981-10-5650-5 |
| DOIs | |
| Publication status | Published - 2018 |
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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.Research output: Contribution in Book/Catalog/Report/Conference proceeding › Chapter (peer-reviewed)
TY - CHAP
T1 - Quantum Chemical Methods for Predicting and Interpreting Second-Order Nonlinear Optical Properties: From Small to Extended π-Conjugated Molecules
AU - Champagne, Benoît
AU - Beaujean, Pierre
AU - De Wergifosse, Marc
AU - Hidalgo Cardenuto, Marcelo
AU - Liégeois, Vincent
AU - Castet, Frédéric
PY - 2018
Y1 - 2018
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.
UR - https://link.springer.com/chapter/10.1007%2F978-981-10-5651-2_6
U2 - 10.1007/978-981-10-5651-2_6
DO - 10.1007/978-981-10-5651-2_6
M3 - Chapter (peer-reviewed)
SN - 978-981-10-5650-5
SP - 117
EP - 138
BT - Frontiers of Quantum Chemistry
A2 - Wojcik, Marek
A2 - Nakatsuji, Hiroshi
A2 - Kirtman, Bernard
A2 - Ozaki, Yokohiro
PB - Springer
CY - Singapore
ER -