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

doi:10.1039/d0cp02992k

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 language	English
Pages (from-to)	16579-16594
Number of pages	16
Journal	PCCP : Physical Chemistry Chemical Physics
Volume	22
Issue number	29
Early online date	8 Jul 2020
DOIs	https://doi.org/10.1039/d0cp02992k
Publication status	Published - 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).

Funders	Funder number
ANR-10-IDEX-03-02
Basque Government/Eusko Jaurlaritza	2019-CIEN-000092-01, PIBA19-0004, PRE-2019-2-0168, IT1254-19
Donostia International Physics Center (DIPC)
FNRS‐FRFC	2.4.617.07
Universitéde Bordeaux
Edge Hill University
Ministerio de Economía y Competitividad	EUIN2017-88605, EUR2019-103825, PGC2018-098212-B-C21
Euskal Herriko Unibertsitatea
Université Montesquieu-Bordeaux IV
Conseil Régional Aquitaine

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10.1039/d0cp02992k

Phys. Chem. Chem. Phys. 22, 16579-16594 (2020)Final published version, 5.81 MB

Cite this

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title = "Performance of DFT functionals for calculating the second-order nonlinear optical properties of dipolar merocyanines",

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 M{\o}ller-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.",

author = "Laurie Lescos and Sitkiewicz, {Sebastian P.} and Pierre Beaujean and Mireille Blanchard-Desce and Beno{\^i}t Champagne and Eduard Matito and Fr{\'e}d{\'e}ric Castet",

note = "Funding Information: 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 Universit{\'e}de 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 M{\'e}socentre de Calcul Intensif Aquitain (MCIA) of the University of Bordeaux and of the Universit{\'e}de Pau et des Pays de l{\textquoteright}Adour and funded by the Conseil R{\'e}gional d{\textquoteright}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. Li{\'e}geois, UNamur, www.unamur.be/drawmol). Publisher Copyright: {\textcopyright} the Owner Societies.",

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AU - Champagne, Benoît

AU - Matito, Eduard

AU - Castet, Frédéric

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N2 - 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.

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

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

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High Performance Computing Technology Platform

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