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Résumé
The Quantum Theory of Atoms in Molecules (QTAIM) to distribute the molecular polarizability tensors over submolecular sites is employed to improve the prediction of local field tensors of molecular crystals and therefore of their linear and secondorder nonlinear optical susceptibilities. This extension of the twostep multiscale procedure is intended to better describe crystals built of molecules having complex shapes. When combined with a simple charge embedding approach to account for the crystal field effects on the molecular (hyper)polarizabilities, this QTAIM local field theory (QLFT) approach is efficient to predict the _{χ} ^{(1)} and _{χ} ^{(2)} tensor components. Moreover, it does not require substantial computational resources because the largest calculations are performed on the individual molecules. This is illustrated by considering derivatives of (S)2(αmethylbenzylamino)5nitropyridine (MBANP) as well as 2methyl4nitroanline (MNA), which is a prototypical pushpull πconjugated compound. In the latter case, the use of the QLFT only leads to minor differences in the _{χ} ^{(1)} and _{χ} ^{(2)} tensor components with respect to the standard approach where the polarizability is equipartitioned. In the case of the MBANP derivatives, the QLFT scheme leads to systematic decrease of the linear and nonlinear optical responses. This generally improves the agreement between the calculated and experimental refractive indices and secondorder nonlinear optical susceptibilities. Indeed, the standard partitioning scheme leads to an overestimation of the phenyl outofplane polarization component and therefore of the refractive indices. The _{χ} ^{(2)} variations among the MBANP derivatives have further been analyzed in terms of molecular geometry, crystal polarizing field, and crystal packing. (Chemical Equation Presented).
langue originale  Anglais 

Pages (de  à)  44814494 
Nombre de pages  14 
journal  Journal of Physical Chemistry C: Nanomaterials and interfaces 
Volume  120 
Numéro de publication  8 
Les DOIs  
Etat de la publication  Publié  3 mars 2016 
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Subvention  Professeur de recherche Francqui
Nakano, M. & Castet, F.
1/09/12 → 31/12/15
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PAI n°P7/05  FS2: Systèmes supramoléculaires fonctionnels (PAI P7/05)
CHAMPAGNE, B., De Vos, D., Van der Auweraer, M., Jérôme, C., Lazzaroni, R., Marin, G., Jonas, A., Du Prez, F., Vanderzande, D., Van Tendeloo, G., Van Speybroeck, V., NENON, S. & STAELENS, N.
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