TY - JOUR
T1 - Performance of DFT functionals for calculating the second-order nonlinear optical properties of dipolar merocyanines
AU - Lescos, Laurie
AU - Sitkiewicz, Sebastian P.
AU - Beaujean, Pierre
AU - Blanchard-Desce, Mireille
AU - Champagne, Benoît
AU - Matito, Eduard
AU - Castet, Frédéric
N1 - 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 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).
Publisher Copyright:
© the Owner Societies.
PY - 2020/8/7
Y1 - 2020/8/7
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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85088879722&partnerID=8YFLogxK
U2 - 10.1039/d0cp02992k
DO - 10.1039/d0cp02992k
M3 - Article
C2 - 32677655
AN - SCOPUS:85088879722
SN - 1463-9076
VL - 22
SP - 16579
EP - 16594
JO - Physical Chemistry Chemical Physics
JF - Physical Chemistry Chemical Physics
IS - 29
ER -