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Fine-tuning polyoxometalate non-linear optical chromophores: a molecular electronic “Goldilocks” effect

Al-Yasari, Ahmed and Spence, Philip and El Moll, Hani and Van Steerteghem, Nick and Horton, Peter N. and Brunschwig, Bruce S. and Clays, Koen and Fielden, John (2018) Fine-tuning polyoxometalate non-linear optical chromophores: a molecular electronic “Goldilocks” effect. Dalton Transactions, 47 (31). pp. 10415-10419. ISSN 1477-9226. https://resolver.caltech.edu/CaltechAUTHORS:20180627-151212518

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Abstract

A new aryl-imido polyoxometalate non-linear optical chromophore (POMophore) with a diphenylamino donor group attains the highest βzzz, 0 value (196 × 10^(−30) esu by Hyper-Rayleigh Scattering, HRS), and best transparency/non-linearity trade off yet for such materials. Stark spectroscopic and DFT investigation of this compound, plus NMe_2 and carbazole analogues, show that its high performance results from a combination of strongly dipolar electronic transitions, and strong electronic communication across the π-system.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://dx.doi.org/10.1039/c8dt01491dDOIArticle
http://www.rsc.org/suppdata/c8/dt/c8dt01491d/c8dt01491d1.pdfPublisherSupporting Information
http://www.rsc.org/suppdata/c8/dt/c8dt01491d/c8dt01491d2.cifPublisherSupporting Information
ORCID:
AuthorORCID
Al-Yasari, Ahmed0000-0001-8768-1248
Spence, Philip0000-0002-3009-2423
Brunschwig, Bruce S.0000-0002-6135-6727
Fielden, John0000-0001-5963-7792
Additional Information:© 2018 The author(s). This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. Received 16th April 2018 , Accepted 15th May 2018. First published on 27th June 2018. We thank the UK EPSRC National Mass Spectrometry Facility for MS. This work was supported by: the Iraqi Government (HCED scholarship to AAY), Royal Society of Chemistry, EPSRC (EP/M00452X/1) and Fonds voor Wetenschappelijk Onderzoek-Vlaanderen (FWO-V, PhD fellowship for NVS). BSB acknowledges support from the Beckman Institute of the California Institute of Technology. Stark data were collected and analysed at the Molecular Materials Resource Center of the Beckman Institute of the California Institute of Technology. In addition to the supplementary information and deposited cif files, data can be accessed by contacting the corresponding author.
Funders:
Funding AgencyGrant Number
Higher Committee For Education Development (Iraq)UNSPECIFIED
Royal Society of ChemistryUNSPECIFIED
Engineering and Physical Sciences Research Council (EPSRC)EP/M00452X/1
Fonds Wetenschappelijk Onderzoek - Vlaanderen (FWO)UNSPECIFIED
Caltech Beckman InstituteUNSPECIFIED
Issue or Number:31
Record Number:CaltechAUTHORS:20180627-151212518
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20180627-151212518
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:87417
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:27 Jun 2018 22:43
Last Modified:03 Oct 2019 19:55

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