Performance of DFT functionals for calculating the second-order nonlinear optical properties of dipolar merocyanines

Laurie Lescos, Sebastian P. Sitkiewicz, Pierre Beaujean, Mireille Blanchard-Desce, Benoît Champagne, Eduard Matito, Frédéric Castet

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Abstract

The second-order nonlinear optical responses of a series of recently designed dipolar merocyanines are investigated using the 2006 Minnesota family of hybrid exchange-correlation functionals (XCFs), as well as the LC-BLYP, ωB97XD and CAM-B3LYP long-range (LR) corrected XCFs. The performance of these different levels of approximation is discussed in regard to reference second-order Møller-Plesset calculations and experimental data obtained from Hyper-Rayleigh Scattering (HRS) measurements. Particular focus is given to the influence of the amount of exact Hartree-Fock exchange included in the XCF on the magnitude of the static HRS responses, as well as to the impact of tuning the range-separation parameter in LR-XCFs, according to a system-specific nonempirical procedure. Frequency dispersion effects are also investigated, as well as their crucial role in the comparison between theoretical and experimental data.

Original languageEnglish
Pages (from-to)16579-16594
Number of pages16
JournalPCCP : Physical Chemistry Chemical Physics
Volume22
Issue number29
Early online date8 Jul 2020
DOIs
Publication statusPublished - 7 Aug 2020

Funding

This work was supported by the Transnational Common Laboratory QuantumChemPhys: Theoretical Chemistry and Physics at the Quantum Scale (ANR-10-IDEX-03-02), between the Universitéde Bordeaux (UBx), Euskal Herriko Unibertsitatea (UPV/EHU) and Donostia International Physics Center (DIPC). This research was also funded by Spanish MINECO grant numbers PGC2018-098212-B-C21, EUIN2017-88605 and EUR2019-103825, the Basque Government/Eusko Jaurlaritza (GV/EJ) grant numbers IT1254-19, PIBA19-0004, 2019-CIEN-000092-01 and PRE-2019-2-0168. Calculations were performed on the computing facilities provided by the Mésocentre de Calcul Intensif Aquitain (MCIA) of the University of Bordeaux and of the Universitéde Pau et des Pays de l’Adour and funded by the Conseil Régional d’Aquitaine, as well as by the Consortium des Equipements de Calcul Intensif (CECI, http://www.ceci-hpc.be), in particular the Technological Platform on High-Performance Computing, financed by the FNRS-FRFC (Conventions No. 2.4.617.07.F and 2.5020.11) and the University of Namur. Unit sphere representations have been generated using the DrawMol software (DrawMol, V. Liégeois, UNamur, www.unamur.be/drawmol).

FundersFunder number
ANR-10-IDEX-03-02
Basque Government/Eusko Jaurlaritza2019-CIEN-000092-01, PIBA19-0004, PRE-2019-2-0168, IT1254-19
Donostia International Physics Center (DIPC)
FNRS‐FRFC2.4.617.07
Universitéde Bordeaux
Edge Hill University
Ministerio de Economía y CompetitividadEUIN2017-88605, EUR2019-103825, PGC2018-098212-B-C21
Euskal Herriko Unibertsitatea
Université Montesquieu-Bordeaux IV
Conseil Régional Aquitaine

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