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Résumé
This review presents the theoretical background concerning simplified quantum chemistry (sQC) methods to compute nonlinear optical (NLO) properties and their applications to large systems. To evaluate any NLO responses such as hyperpolarizabilities or twophoton absorption (2PA), one should evidently perform first a ground state calculation and compute its response. Because of this, methods used to compute ground states of large systems are outlined, especially the xTB (extended tightbinding) scheme. An overview on approaches to compute excited state and response properties is given, emphasizing the simplified timedependent density functional theory (sTDDFT). The formalism of the eXact integral sTDDFT (XsTDDFT) method is also introduced. For the first hyperpolarizability, 2PA, excited state absorption, and second hyperpolarizability, a brief historical review is given on earlystage semiempirical method applications to systems that were considered large at the time. Then, we showcase recent applications with sQC methods, especially the sTDDFT scheme to large challenging systems such as fluorescent proteins or fluorescent organic nanoparticles as well as dynamic structural effects on flexible tryptophanrich peptides and gramicidin A. Thanks to the sTDDFTxTB scheme, allatom quantum chemistry methodologies are now possible for the computation of the first hyperpolarizability and 2PA of systems up to 5000 atoms. This review concludes by summingup current and future method developments in the sQC framework as well as forthcoming applications on large systems. This article is categorized under: Electronic Structure Theory > Ab Initio Electronic Structure Methods Structure and Mechanism > Molecular Structures Electronic Structure Theory > Density Functional Theory Electronic Structure Theory > Semiempirical Electronic Structure Methods.
langue originale  Anglais 

Numéro d'article  e1695 
journal  Wiley Interdisciplinary Reviews: Computational Molecular Science 
Volume  14 
Numéro de publication  1 
Les DOIs  
Etat de la publication  Publié  1 janv. 2024 
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CÉCI – Consortium des Équipements de Calcul Intensif
Champagne, B., Lazzaroni, R., Geuzaine , C., Chatelain, P. & Knaepen, B.
1/01/18 → 31/12/22
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Plateforme Technologique Calcul Intensif
Benoît Champagne (!!Manager)
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