Electrochemically-switched 2nd order non-linear optical response in an arylimido-polyoxometalate with high contrast and cyclability

Bethany Rose Hood; Yovan de Coene; Afonso Vieira Torre Do Vale Froes; Claire Jones; Pierre Beaujean; Vincent Liegois; Fraser MacMillan; Benoit 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 Rose Hood
, Yovan de Coene
, Afonso Vieira Torre Do Vale Froes
, Claire Jones
, Pierre Beaujean
, Vincent Liegois
, Fraser MacMillan
, Benoit Champagne
, Koen Clays
, John Fielden

Centre for Molecular and Structural Biochemistry

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

8 Citations (Scopus)

43 Downloads (Pure)

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.

Original language	English
Article number	e202215537
Journal	Angewandte Chemie-International Edition
Volume	62
Issue number	5
Early online date	30 Nov 2022
DOIs	https://doi.org/10.1002/anie.202215537
Publication status	Published - 26 Jan 2023

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10.1002/anie.202215537Licence: CC BY

Angew Chem Int Ed - 2022 - Hood - Electrochemically‐Switched 2nd Order Non‐Linear Optical Response in anAccepted author manuscript, 949 KBLicence: CC BY

Enhanced single-crystal X-ray diffraction facilities
Bochmann, M. (Principal Investigator), Fabian, L. (Co-Investigator), Fielden, J. (Co-Investigator), Khimyak, Y. (Co-Investigator) & Wright, J. (Co-Investigator)
Engineering and Physical Sciences Research Council
15/11/18 → 14/11/21
Project: Research
Polyoxometalate-Based Sensitizers for p-Type Dye-Sensitized Solar Cells
Fielden, J. (Principal Investigator)
Engineering and Physical Sciences Research Council
31/12/14 → 29/06/16
Project: Research

Cite this

Hood, B. R., de Coene, Y., Vieira Torre Do Vale Froes, A., Jones, C., Beaujean, P., Liegois, 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

@article{8888309dd22e405eb6001a57238ef62f,

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.",

author = "Hood, \{Bethany Rose\} and \{de Coene\}, Yovan and \{Vieira Torre Do Vale Froes\}, Afonso and Claire Jones and Pierre Beaujean and Vincent Liegois and Fraser MacMillan and Benoit Champagne and Koen Clays and John Fielden",

note = "Research Funding: Engineering and Physical Sciences Research Council. Grant Numbers: EP/M00452X/1, EP/S005854/1; University of East Anglia. Grant Numbers: Studentship, Katritzky Scholarship; Leverhulme Trust. Grant Number: RPG-2020-365; Royal Society. Grant Number: Woolfson Research Merit Award; Fonds Wetenschappelijk Onderzoek. Grant Number: 1234222N; FRS-FNRS. Grant Number: Research Associate; FNRS-FRFC. Grant Number: U.G018.19, U.G011.22, RW/GEQ2016, GEQ U.G011.22; Walloon Region. Grant Number: 1610468, RW/GEQ2016, 2110213",

year = "2023",

month = jan,

day = "26",

doi = "10.1002/anie.202215537",

language = "English",

volume = "62",

journal = "Angewandte Chemie-International Edition",

issn = "1433-7851",

publisher = "Wiley",

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Hood, BR, de Coene, Y, Vieira Torre Do Vale Froes, A, Jones, C, Beaujean, P, Liegois, 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

TY - JOUR

T1 - Electrochemically-switched 2nd order non-linear optical response in an arylimido-polyoxometalate with high contrast and cyclability

AU - Hood, Bethany Rose

AU - de Coene, Yovan

AU - Vieira Torre Do Vale Froes, Afonso

AU - Jones, Claire

AU - Beaujean, Pierre

AU - Liegois, Vincent

AU - MacMillan, Fraser

AU - Champagne, Benoit

AU - Clays, Koen

AU - Fielden, John

N1 - Research Funding: Engineering and Physical Sciences Research Council. Grant Numbers: EP/M00452X/1, EP/S005854/1; University of East Anglia. Grant Numbers: Studentship, Katritzky Scholarship; Leverhulme Trust. Grant Number: RPG-2020-365; Royal Society. Grant Number: Woolfson Research Merit Award; Fonds Wetenschappelijk Onderzoek. Grant Number: 1234222N; FRS-FNRS. Grant Number: Research Associate; FNRS-FRFC. Grant Number: U.G018.19, U.G011.22, RW/GEQ2016, GEQ U.G011.22; Walloon Region. Grant Number: 1610468, RW/GEQ2016, 2110213

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.

U2 - 10.1002/anie.202215537

DO - 10.1002/anie.202215537

M3 - Article

SN - 1433-7851

VL - 62

JO - Angewandte Chemie-International Edition

JF - Angewandte Chemie-International Edition

IS - 5

M1 - e202215537

ER -

Electrochemically-switched 2nd order non-linear optical response in an arylimido-polyoxometalate with high contrast and cyclability

Abstract

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Projects

Enhanced single-crystal X-ray diffraction facilities

Polyoxometalate-Based Sensitizers for p-Type Dye-Sensitized Solar Cells

Cite this