Electrochemically-Switched 2nd Order Non-Linear Optical Response in an Arylimido-Polyoxometalate with High Contrast and Cyclability

Bethany R. Hood; Yovan de Coene; Afonso V. Torre Do Vale Froes; Claire F. Jones; Pierre Beaujean; Vincent Liégeois; Fraser MacMillan; Benoît Champagne; Koen Clays; John Fielden

doi:10.1002/anie.202215537

Electrochemically-Switched 2nd Order Non-Linear Optical Response in an Arylimido-Polyoxometalate with High Contrast and Cyclability

Bethany R. Hood, Yovan de Coene, Afonso V. Torre Do Vale Froes, Claire F. Jones, Pierre Beaujean, Vincent Liégeois, Fraser MacMillan, Benoît Champagne, Koen Clays, John Fielden

University of Namur

Research output: Contribution to journal › Article › peer-review

Abstract

Electrochemically switched 2^nd order non-linear optical responses have been demonstrated for the first time in polyoxometalates (POMs), with an arylimido-derivative showing a leading combination of high on/off contrast (94 %), high visible transparency, and cyclability. Spectro-electrochemical and TD-DFT studies indicate that the switch-off results from weakened charge transfer (CT) character of the electronic transitions in the reduced state. This represents the first study of an imido-POM reduced state, and demonstrates the potential of POM hybrids as electrochemically activated molecular switches.

Original language	English
Article number	e202215537
Number of pages	5
Journal	Angewandte Chemie - International Edition
Volume	62
Issue number	5
DOIs	https://doi.org/10.1002/anie.202215537
Publication status	Published - 26 Jan 2023

Keywords

Donor-Acceptor Systems
Molecular Devices
Nonlinear Optics
Polyoxometalates
Spectroelectrochemistry

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10.1002/anie.202215537

Cite this

Hood, B. R., de Coene, Y., Torre Do Vale Froes, A. V., Jones, C. F., Beaujean, P., Liégeois, V., MacMillan, F., Champagne, B., Clays, K., & Fielden, J. (2023). Electrochemically-Switched 2nd Order Non-Linear Optical Response in an Arylimido-Polyoxometalate with High Contrast and Cyclability. Angewandte Chemie - International Edition, 62(5), Article e202215537. https://doi.org/10.1002/anie.202215537

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title = "Electrochemically-Switched 2nd Order Non-Linear Optical Response in an Arylimido-Polyoxometalate with High Contrast and Cyclability",

abstract = "Electrochemically switched 2nd order non-linear optical responses have been demonstrated for the first time in polyoxometalates (POMs), with an arylimido-derivative showing a leading combination of high on/off contrast (94 %), high visible transparency, and cyclability. Spectro-electrochemical and TD-DFT studies indicate that the switch-off results from weakened charge transfer (CT) character of the electronic transitions in the reduced state. This represents the first study of an imido-POM reduced state, and demonstrates the potential of POM hybrids as electrochemically activated molecular switches.",

keywords = "Donor-Acceptor Systems, Molecular Devices, Nonlinear Optics, Polyoxometalates, Spectroelectrochemistry",

author = "Hood, {Bethany R.} and {de Coene}, Yovan and {Torre Do Vale Froes}, {Afonso V.} and Jones, {Claire F.} and Pierre Beaujean and Vincent Li{\'e}geois and Fraser MacMillan and Beno{\^i}t Champagne and Koen Clays and John Fielden",

note = "Publisher Copyright: {\textcopyright} 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.",

year = "2023",

month = jan,

day = "26",

doi = "10.1002/anie.202215537",

language = "English",

volume = "62",

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Hood, BR, de Coene, Y, Torre Do Vale Froes, AV, Jones, CF, Beaujean, P , Liégeois, V, MacMillan, F, Champagne, B, Clays, K & Fielden, J 2023, 'Electrochemically-Switched 2nd Order Non-Linear Optical Response in an Arylimido-Polyoxometalate with High Contrast and Cyclability', Angewandte Chemie - International Edition, vol. 62, no. 5, e202215537. https://doi.org/10.1002/anie.202215537

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T1 - Electrochemically-Switched 2nd Order Non-Linear Optical Response in an Arylimido-Polyoxometalate with High Contrast and Cyclability

AU - Hood, Bethany R.

AU - de Coene, Yovan

AU - Torre Do Vale Froes, Afonso V.

AU - Jones, Claire F.

AU - Beaujean, Pierre

AU - Liégeois, Vincent

AU - MacMillan, Fraser

AU - Champagne, Benoît

AU - Clays, Koen

AU - Fielden, John

PY - 2023/1/26

Y1 - 2023/1/26

N2 - Electrochemically switched 2nd order non-linear optical responses have been demonstrated for the first time in polyoxometalates (POMs), with an arylimido-derivative showing a leading combination of high on/off contrast (94 %), high visible transparency, and cyclability. Spectro-electrochemical and TD-DFT studies indicate that the switch-off results from weakened charge transfer (CT) character of the electronic transitions in the reduced state. This represents the first study of an imido-POM reduced state, and demonstrates the potential of POM hybrids as electrochemically activated molecular switches.

AB - Electrochemically switched 2nd order non-linear optical responses have been demonstrated for the first time in polyoxometalates (POMs), with an arylimido-derivative showing a leading combination of high on/off contrast (94 %), high visible transparency, and cyclability. Spectro-electrochemical and TD-DFT studies indicate that the switch-off results from weakened charge transfer (CT) character of the electronic transitions in the reduced state. This represents the first study of an imido-POM reduced state, and demonstrates the potential of POM hybrids as electrochemically activated molecular switches.

KW - Donor-Acceptor Systems

KW - Molecular Devices

KW - Nonlinear Optics

KW - Polyoxometalates

KW - Spectroelectrochemistry

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U2 - 10.1002/anie.202215537

DO - 10.1002/anie.202215537

M3 - Article

AN - SCOPUS:85144830971

SN - 1433-7851

VL - 62

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 5

M1 - e202215537

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Electrochemically-Switched 2nd Order Non-Linear Optical Response in an Arylimido-Polyoxometalate with High Contrast and Cyclability

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Electrochemically-Switched 2nd Order Non-Linear Optical Response in an Arylimido-Polyoxometalate with High Contrast and Cyclability

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Keywords

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Equipment renewal for the Consortium des Equipements de Calcul Intensif (CECI)

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