Salicylideneaniline-Based Covalent Organic Frameworks: A New Family of Multistate Second-Order Nonlinear Optical Switches

Jean Quertinmont; Lorenzo Maschio; Ayan Datta; Benoît Champagne

doi:10.1021/acs.jpcc.0c07672

Salicylideneaniline-Based Covalent Organic Frameworks: A New Family of Multistate Second-Order Nonlinear Optical Switches

Jean Quertinmont, Lorenzo Maschio, Ayan Datta, Benoît Champagne

Résultats de recherche: Contribution à un journal/une revue › Article › Revue par des pairs

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Résumé

This work demonstrates that covalent organic frameworks (COFs) can exhibit large second-order nonlinear (NLO) responses and that these NLO responses can be modulated as a function of successive enol-imine/keto-enamine tautomerisms, leading to efficient solid-state second-order NLO switches. The proof of concept is given by evidencing, by means of periodic boundary condition (time-dependent) density functional theory calculations, the large amplitudes of the second-order NLO susceptibility, χ(2), of two-dimensional COFs built from the assembly of tris(N-salicylideneaniline) units as well as their variations when switching between keto and enol forms. Calculations further demonstrate the key role of symmetry, that is, the distribution of enol and keto functions in the unit cell, on the χ(2) values as well as on their dipolar/octupolar character.

langue originale	Anglais
Pages (de - à)	24451-24459
Nombre de pages	9
journal	Journal of Physical Chemistry C
Volume	124
Numéro de publication	44
Les DOIs	https://doi.org/10.1021/acs.jpcc.0c07672
Etat de la publication	Publié - 5 nov. 2020

Accès au document

10.1021/acs.jpcc.0c07672

J. Phys. Chem. C 124, 24451-24459 (2020)Version finale publiée, 1,2 MB

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Link to publication in Scopus

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
OPTICAL PROPERTIES OF MOFS/COFS: Computational Investigations for the Linear and Nonlinear Optical Properties of Metal and Covalent Organic Frameworks: Applications for Detection of Molecules
CHAMPAGNE, B. & Datta, A.
1/01/18 → 31/12/21
Projet: Recherche
ARC 15/20-068: Improving the Photochromism and Thermochromism in the Solid State by Co-crystallization : an Integrated Physico-chemical Approach
CHAMPAGNE, B., Wouters, J. & Leyssens, T.
1/09/15 → 31/12/20
Projet: Recherche

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

Contient cette citation

@article{f80e6d83fc5f4abcafaf655cfeb2619e,

title = "Salicylideneaniline-Based Covalent Organic Frameworks: A New Family of Multistate Second-Order Nonlinear Optical Switches",

abstract = "This work demonstrates that covalent organic frameworks (COFs) can exhibit large second-order nonlinear (NLO) responses and that these NLO responses can be modulated as a function of successive enol-imine/keto-enamine tautomerisms, leading to efficient solid-state second-order NLO switches. The proof of concept is given by evidencing, by means of periodic boundary condition (time-dependent) density functional theory calculations, the large amplitudes of the second-order NLO susceptibility, χ(2), of two-dimensional COFs built from the assembly of tris(N-salicylideneaniline) units as well as their variations when switching between keto and enol forms. Calculations further demonstrate the key role of symmetry, that is, the distribution of enol and keto functions in the unit cell, on the χ(2) values as well as on their dipolar/octupolar character.",

author = "Jean Quertinmont and Lorenzo Maschio and Ayan Datta and Beno{\^i}t Champagne",

note = "Funding Information: J.Q. thanks the “Actions de Recherche Concert{\'e}es” (ARC) de la Direction g{\'e}n{\'e}rale de l{\textquoteright}Enseignement non obligatoire et de la Recherche scientifique—Direction de la Recherche scientifique—Communaut{\'e} fran{\c c}aise de Belgique, under convention no. 15/20-068 for his PhD grant. J.Q., A.D., and B.C thank BELSPO for fundings through the Indo-Belgian Research and Technology Cooperation project BL/13/IN16 entitled “Optical Properties of MOFS/COFS”. The authors thank N. Mandal for preliminary investigations on this topic. The calculations were performed on the computers of the Consortium des {\'E}quipements de Calcul Intensif (C{\'E}CI, http://www.ceci-hpc.be ) and particularly those of the Technological Platform of High-Performance Computing, for which the authors gratefully acknowledge the financial support of the FNRS-FRFC, of the Walloon Region, and of the University of Namur (Conventions no. 2.5020.11, GEQ U.G006.15, 1610468, and RW/GEQ2016), as well as of zenobe, the Tier-1 facility of the Walloon Region (Convention 1117545). Publisher Copyright: {\textcopyright} 2020 American Chemical Society. Copyright: Copyright 2020 Elsevier B.V., All rights reserved.",

year = "2020",

month = nov,

day = "5",

doi = "10.1021/acs.jpcc.0c07672",

language = "English",

volume = "124",

pages = "24451--24459",

journal = "Journal of physical chemistry. C",

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publisher = "American Chemical Society",

number = "44",

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T1 - Salicylideneaniline-Based Covalent Organic Frameworks

T2 - A New Family of Multistate Second-Order Nonlinear Optical Switches

AU - Quertinmont, Jean

AU - Maschio, Lorenzo

AU - Datta, Ayan

AU - Champagne, Benoît

N1 - Funding Information: J.Q. thanks the “Actions de Recherche Concertées” (ARC) de la Direction générale de l’Enseignement non obligatoire et de la Recherche scientifique—Direction de la Recherche scientifique—Communauté française de Belgique, under convention no. 15/20-068 for his PhD grant. J.Q., A.D., and B.C thank BELSPO for fundings through the Indo-Belgian Research and Technology Cooperation project BL/13/IN16 entitled “Optical Properties of MOFS/COFS”. The authors thank N. Mandal for preliminary investigations on this topic. The calculations were performed on the computers of the Consortium des Équipements de Calcul Intensif (CÉCI, http://www.ceci-hpc.be ) and particularly those of the Technological Platform of High-Performance Computing, for which the authors gratefully acknowledge the financial support of the FNRS-FRFC, of the Walloon Region, and of the University of Namur (Conventions no. 2.5020.11, GEQ U.G006.15, 1610468, and RW/GEQ2016), as well as of zenobe, the Tier-1 facility of the Walloon Region (Convention 1117545). Publisher Copyright: © 2020 American Chemical Society. Copyright: Copyright 2020 Elsevier B.V., All rights reserved.

PY - 2020/11/5

Y1 - 2020/11/5

N2 - This work demonstrates that covalent organic frameworks (COFs) can exhibit large second-order nonlinear (NLO) responses and that these NLO responses can be modulated as a function of successive enol-imine/keto-enamine tautomerisms, leading to efficient solid-state second-order NLO switches. The proof of concept is given by evidencing, by means of periodic boundary condition (time-dependent) density functional theory calculations, the large amplitudes of the second-order NLO susceptibility, χ(2), of two-dimensional COFs built from the assembly of tris(N-salicylideneaniline) units as well as their variations when switching between keto and enol forms. Calculations further demonstrate the key role of symmetry, that is, the distribution of enol and keto functions in the unit cell, on the χ(2) values as well as on their dipolar/octupolar character.

AB - This work demonstrates that covalent organic frameworks (COFs) can exhibit large second-order nonlinear (NLO) responses and that these NLO responses can be modulated as a function of successive enol-imine/keto-enamine tautomerisms, leading to efficient solid-state second-order NLO switches. The proof of concept is given by evidencing, by means of periodic boundary condition (time-dependent) density functional theory calculations, the large amplitudes of the second-order NLO susceptibility, χ(2), of two-dimensional COFs built from the assembly of tris(N-salicylideneaniline) units as well as their variations when switching between keto and enol forms. Calculations further demonstrate the key role of symmetry, that is, the distribution of enol and keto functions in the unit cell, on the χ(2) values as well as on their dipolar/octupolar character.

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DO - 10.1021/acs.jpcc.0c07672

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VL - 124

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JO - Journal of physical chemistry. C

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ER -

Salicylideneaniline-Based Covalent Organic Frameworks: A New Family of Multistate Second-Order Nonlinear Optical Switches

Résumé

Accès au document

Autres fichiers et liens

Empreinte digitale

Projets

CÉCI – Consortium des Équipements de Calcul Intensif

OPTICAL PROPERTIES OF MOFS/COFS: Computational Investigations for the Linear and Nonlinear Optical Properties of Metal and Covalent Organic Frameworks: Applications for Detection of Molecules

ARC 15/20-068: Improving the Photochromism and Thermochromism in the Solid State by Co-crystallization : an Integrated Physico-chemical Approach

Équipement

Plateforme Technologique Calcul Intensif

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