Nonlinear optical switching behavior in the solid state: A theoretical investigation on anils

Handle URI:
http://hdl.handle.net/10754/561874
Title:
Nonlinear optical switching behavior in the solid state: A theoretical investigation on anils
Authors:
Ségerie, Audrey; Castet, Frédéric; Kanoun, Mohammed; Plaquet, Aurélie; Liégeois, Vincent; Champagne, Benoit
Abstract:
The linear (π(1)) and second-order nonlinear (π(2)) optical properties of two anil crystals, [N-(4-hydroxy)-salicylidene-amino-4-(methylbenzoate) and N-(3,5-di-tert- butylsalicylidene)-4-aminopyridine, denoted 4A and 4P, respectively], as well as the optical contrasts upon switching between their enol (E) and keto (K) forms, have been investigated by combining the molecular responses calculated using quantum chemistry methods and an electrostatic interaction scheme to account for the local field effects. It is found that intermolecular interactions impact differently the K/E optical contrasts in the two systems, which illustrates the importance of the supramolecular organization on the macroscopic responses. In 4A, the surrounding effects on the (hyper)polarizabilities are similar in the enol and keto forms, leading to optical contrasts very close to those of the isolated molecule. In contrast, an enhancement of the second-order susceptibility is observed in the keto form of 4P, leading to a large π(2)(K)/π(2)(E) contrast. Moreover, the π(2)(4A)/π(2)(4P) ratio for the most stable enol forms is obtained to be in good agreement with previous experimental investigations, which supports the reliability of the computational procedure. © 2011 American Chemical Society.
KAUST Department:
Physical Sciences and Engineering (PSE) Division; KAUST Catalysis Center (KCC)
Publisher:
American Chemical Society
Journal:
Chemistry of Materials
Issue Date:
13-Sep-2011
DOI:
10.1021/cm2015516
Type:
Article
ISSN:
08974756
Appears in Collections:
Articles; Physical Sciences and Engineering (PSE) Division; KAUST Catalysis Center (KCC)

Full metadata record

DC FieldValue Language
dc.contributor.authorSégerie, Audreyen
dc.contributor.authorCastet, Frédéricen
dc.contributor.authorKanoun, Mohammeden
dc.contributor.authorPlaquet, Aurélieen
dc.contributor.authorLiégeois, Vincenten
dc.contributor.authorChampagne, Benoiten
dc.date.accessioned2015-08-03T09:33:00Zen
dc.date.available2015-08-03T09:33:00Zen
dc.date.issued2011-09-13en
dc.identifier.issn08974756en
dc.identifier.doi10.1021/cm2015516en
dc.identifier.urihttp://hdl.handle.net/10754/561874en
dc.description.abstractThe linear (π(1)) and second-order nonlinear (π(2)) optical properties of two anil crystals, [N-(4-hydroxy)-salicylidene-amino-4-(methylbenzoate) and N-(3,5-di-tert- butylsalicylidene)-4-aminopyridine, denoted 4A and 4P, respectively], as well as the optical contrasts upon switching between their enol (E) and keto (K) forms, have been investigated by combining the molecular responses calculated using quantum chemistry methods and an electrostatic interaction scheme to account for the local field effects. It is found that intermolecular interactions impact differently the K/E optical contrasts in the two systems, which illustrates the importance of the supramolecular organization on the macroscopic responses. In 4A, the surrounding effects on the (hyper)polarizabilities are similar in the enol and keto forms, leading to optical contrasts very close to those of the isolated molecule. In contrast, an enhancement of the second-order susceptibility is observed in the keto form of 4P, leading to a large π(2)(K)/π(2)(E) contrast. Moreover, the π(2)(4A)/π(2)(4P) ratio for the most stable enol forms is obtained to be in good agreement with previous experimental investigations, which supports the reliability of the computational procedure. © 2011 American Chemical Society.en
dc.publisherAmerican Chemical Societyen
dc.subjectelectrostatic interaction schemesen
dc.subjectfirst hyperpolarizabilitiesen
dc.subjectketo-enol molecular switchesen
dc.subjectNonlinear opticsen
dc.subjectorganic molecular crystalsen
dc.subjectquantum chemical calculationsen
dc.subjectsecond-order nonlinear optical susceptibilitiesen
dc.titleNonlinear optical switching behavior in the solid state: A theoretical investigation on anilsen
dc.typeArticleen
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentKAUST Catalysis Center (KCC)en
dc.identifier.journalChemistry of Materialsen
dc.contributor.institutionUniversité de Bordeaux, Institut des Sciences Moléculaires, UMR 5255 CNRS, cours de la Libération, 351, F-33405 Talence, Franceen
dc.contributor.institutionLaboratoire de Chimie Théorique, Unité de Chimie Physique Théorique et Structurale, Facultés Universitaires Notre-Dame de la Paix (FUNDP), rue de Bruxelles 61, B-5000 Namur, Belgiumen
kaust.authorKanoun, Mohammeden
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