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Jones, Claire F. 
ORCID: https://orcid.org/0009-0006-4449-3451, Hood, Bethany, de Coene, Yovan, Kearns, Hayleigh, Faulds, Karen, Champagne, Benoît, Clays, Koen and Fielden, John
(2026)
Electrochemical Switch‐On of Nonlinear Optical Response in a Nitro‐Functionalized Arylimido‐Polyoxometalate.
Angewandte Chemie International Edition.
ISSN 1433-7851
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Abstract
Electrochemical switch-on of second-order non-linear optical (NLO) responses (β) has been demonstrated in a polyoxometalate (POM) based chromophore (POMophore) for the first time. Reduction of the POM in a POM-imidoaryl-NO 2 derivative invokes an up to 15-fold off/on switchable increase in intensity of scattered frequency-doubled light, and the highest “on” state β yet reported for a redox-cyclable POMophore. Computational and spectroscopic studies show that in the oxidized state, directionally opposed charge transfer (CT) transitions to POM and ─NO 2 result in a low net β. Upon reduction, the POM becomes a much weaker CT acceptor, resulting in more dipolar imido-aryl to nitro CT, and thus enhanced NLO response.
| Item Type: | Article |
|---|---|
| Additional Information: | Data Availability Statement: Data supporting this paper are presented in the supplementary information and will be deposited at DOI: 10.17635/Lancaster/researchdata/278.The CIF file for the structure of [NBu 4 ]2 [1] is available from the CCDC (deposition number 2523544) via https://www.ccdc.cam.ac.uk/structures/. |
| Uncontrolled Keywords: | donor-acceptor systems,molecular switches,nonlinear optics,polyoxometalates,spectroelectrochemistry,catalysis,general chemistry ,/dk/atira/pure/subjectarea/asjc/1500/1503 |
| Faculty \ School: | Faculty of Science > School of Chemistry, Pharmacy and Pharmacology |
| Related URLs: | |
| Depositing User: | LivePure Connector |
| Date Deposited: | 07 Aug 2026 12:18 |
| Last Modified: | 09 Aug 2026 05:43 |
| URI: | https://ueaeprints.uea.ac.uk/id/eprint/104041 |
| DOI: | 10.1002/ANIE.4949539 |
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