Projets par an
Résumé
The electric fieldinduced second harmonic generation (EFISHG) response has been largely used to describe the first β and the second γ hyperpolarizabilities in solution. Although the EFISHG technique cannot be applied to charged compounds (due to the external static electric field), it can be used to describe ion pairs as neutral complexes. A multiscale computational approach is required to generate representative geometrical configurations of such kinds of complexes (using classical force fields), to compute the electronic structure of each configuration (using quantum mechanics methods), and to perform statistical analyses describing the behavior of the nonlinear optical properties. In this work, we target solvated neutral ion pairs complexes, of which the cation is an organic chromophore, and we estimate their EFISHG and hyperRayleigh scattering responses. It is shown that the anion–cation relative spatial distribution determines the permanent dipole moment of the complexes, and therefore the relative distance controls the EFISHG response. On the other hand, the β tensor is independent of the dipole moment and it shows a weak linear correlation with the πelectron conjugation length of the cations. The γ contributions in the global EFISHG response range from 5% to 15%, which is mostly due to the variations of amplitude of the μβ∥ contribution, which results from differences in the μ and β vectors’ orientations. The applied multiscale approach provides reasonable results compared with experimental ones, although additional efforts are still required to improve such comparison mainly to consider the possible dissociation effects.
langue originale  Anglais 

Pages (de  à)  48174826 
Nombre de pages  10 
journal  Journal of chemical information and modeling 
Volume  60 
Numéro de publication  10 
Les DOIs  
Etat de la publication  Publié  26 oct. 2020 
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Projets
 1 Actif

CÉCI – Consortium des Équipements de Calcul Intensif
CHAMPAGNE, B., Lazzaroni, R., Geuzaine , C., Chatelain, P. & Knaepen, B.
1/01/18 → 31/12/22
Projet: Recherche
Équipement

Plateforme Technologique Calcul Intensif
Benoît Champagne (!!Manager)
Plateforme technologique Calcul intensifEquipement/installations: Plateforme technolgique