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Résumé
Using the CRYSTAL17 package at the coupledperturbed KohnSham (CPKS) level, periodic boundary conditions firstprinciples calculations are enacted to predict the second harmonic generation secondorder nonlinear optical (NLO) susceptibility, χ(2), values of six historical NLO crystals. This selection allowed the comparison between stateoftheart calculations and experiment. Several computational aspects are tackled to define conditions where the results are converged with respect to the range of lattice summations, to the number of kpoints in the first Brillouin zone, to the order of the multipole expansions for evaluating the longrange part of the electrostatic interactions, as well as to the atomic basis set size. A valence triple zeta basis set supplemented with polarization functions has been selected. Then, χ(2) calculations have been performed using a range of exchangecorrelation functionals (XCFs). Results show the large impact of the amount of HartreeFock (HF) exchange on the amplitude but also on the sign on the χ(2) tensor components. To a given extent, these amplitude effects are consistent with results on molecules, but the sign reversal effects and the nonmonotonic behavior of the χ(2) tensor components as a function of the amount of HF exchange are scarcely found for molecules. Then, using the recommended rangeseparated hybrid XCFs, the CPKS scheme leads to good agreement with experimental data for potassium dihydrogenophosphate, urea, and χZXX(2) of LiNbO3. The agreement is more questionable for χZZZ(2) of LiNbO3 whereas it remains poor for ammonium dihydrogenophosphate and 2methyl4nitroaniline, with large underestimations by about a factor of 3, opening a path to further finetuning of the ranges of inclusion of HF exchange.
langue originale  Anglais 

Numéro d'article  064707 
Pages (de  à)  064707 
Nombre de pages  14 
journal  The Journal of chemical physics 
Volume  158 
Numéro de publication  6 
Les DOIs  
Etat de la publication  Publié  14 févr. 2023 
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Examiner les sujets de recherche de « Firstprinciples evaluation of the second harmonic generation response of reference organic and inorganic crystals ». Ensemble, ils forment une empreinte digitale unique.Projets
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Quantum Chemical Investigations of the Organic and Organometallic Crystalline Solid State – Design of Materials with Outstanding Electronic, Electrical, Optical, and ElectroOptical Properties
Mairesse, F. (Responsable du Projet) & CHAMPAGNE, B. (Promoteur)
1/10/20 → 1/10/26
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Plateforme Technologique Calcul Intensif
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