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

Résultats de recherche: Contribution à un journal/une revueArticle

Résumé

The linear (π ) and second-order nonlinear (π ) 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 (K)/π (E) contrast. Moreover, the π (4A)/π (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.
langue originaleAnglais
Pages (de - à)3993-4001
Nombre de pages9
journalChemistry of Materials
Volume23
Numéro de publication17
Les DOIs
étatPublié - 13 sept. 2011

Empreinte digitale

Quantum chemistry
4-Aminopyridine
Coulomb interactions
Optical properties
Crystals
Molecules
4-toluic acid

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title = "Nonlinear optical switching behavior in the solid state: A theoretical investigation on anils",
abstract = "The linear (π ) and second-order nonlinear (π ) 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 (K)/π (E) contrast. Moreover, the π (4A)/π (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.",
author = "A. S{\'e}gerie and F. Castet and M.B. Kanoun and A. Plaquet and V. Li{\'e}geois and B. Champagne",
note = "Copyright 2011 Elsevier B.V., All rights reserved.",
year = "2011",
month = "9",
day = "13",
doi = "10.1021/cm2015516",
language = "English",
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pages = "3993--4001",
journal = "Chemistry of Materials",
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Nonlinear optical switching behavior in the solid state : A theoretical investigation on anils. / Ségerie, A.; Castet, F.; Kanoun, M.B.; Plaquet, A.; Liégeois, V.; Champagne, B.

Dans: Chemistry of Materials, Vol 23, Numéro 17, 13.09.2011, p. 3993-4001.

Résultats de recherche: Contribution à un journal/une revueArticle

TY - JOUR

T1 - Nonlinear optical switching behavior in the solid state

T2 - A theoretical investigation on anils

AU - Ségerie, A.

AU - Castet, F.

AU - Kanoun, M.B.

AU - Plaquet, A.

AU - Liégeois, V.

AU - Champagne, B.

N1 - Copyright 2011 Elsevier B.V., All rights reserved.

PY - 2011/9/13

Y1 - 2011/9/13

N2 - The linear (π ) and second-order nonlinear (π ) 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 (K)/π (E) contrast. Moreover, the π (4A)/π (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.

AB - The linear (π ) and second-order nonlinear (π ) 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 (K)/π (E) contrast. Moreover, the π (4A)/π (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.

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