Supramolecular Metal Halide Complexes for High-Temperature Non-linear Optical Switches

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dc.contributor.authorWang, Qianen
dc.contributor.authorJin, Jianboen
dc.contributor.authorWang, Zhongxuanen
dc.contributor.authorRen, Shenqiangen
dc.contributor.authorYe, Qingyuen
dc.contributor.authorDou, Yixuanen
dc.contributor.authorLiu, Sunhaoen
dc.contributor.authorMorris, Amandaen
dc.contributor.authorSlebodnick, Carlaen
dc.contributor.authorQuan, Linaen
dc.date.accessioned2025-02-17T17:38:10Zen
dc.date.available2025-02-17T17:38:10Zen
dc.date.issued2024-02-23en
dc.description.abstractNonlinear optical (NLO) switching materials, which exhibit reversible intensity modulation in response to thermal stimuli, have found extensive applications across diverse fields including sensing, photoelectronics, and photonic applications. While significant progress has been made in solid-state NLO switching materials, these materials typically showcase their highest NLO performance near room temperature. However, this performance drastically deteriorates upon heating, primarily due to the phase transition undergone by the materials from noncentrosymmetric to centrosymmetric phase. Here, we introduce a new class of NLO switching materials, solid-state supramolecular compounds 18-Crown-6 ether@Cu2Cl4·4H2O (1·4H2O), exhibiting reversible and stable NLO switching when subjected to near-infrared (NIR) photoexcitation and/or thermal stimuli. The reversible crystal structure in response to external stimuli is attributed to the presence of a weakly coordinated bridging water molecule facilitated by hydrogen bonding/chelation interactions between the metal halide and crown-ether supramolecules. We observed an exceptionally high second-harmonic generation (SHG) signal under continuous photoexcitation, even at temperatures exceeding 110 °C. In addition, the bridging water molecules within the complex can be released and recaptured in a fully reversible manner, all without requiring excessive energy input. This feature allows for precise control of SHG signal activation and deactivation through structural transformations, resulting in a high-contrast off/on ratio, reaching values in the million-fold range.en
dc.description.versionPublished versionen
dc.format.extentPages 8971-8980en
dc.format.extent10 page(s)en
dc.format.mimetypeapplication/pdfen
dc.identifier.doihttps://doi.org/10.1021/jacs.3c13079en
dc.identifier.eissn1520-5126en
dc.identifier.issn0002-7863en
dc.identifier.issue13en
dc.identifier.orcidMorris, Amanda [0000-0002-3512-0366]en
dc.identifier.orcidSlebodnick, Carla [0000-0003-4188-7595]en
dc.identifier.orcidQuan, Lina [0000-0001-9301-3764]en
dc.identifier.pmid38393312en
dc.identifier.urihttps://hdl.handle.net/10919/124601en
dc.identifier.volume146en
dc.language.isoenen
dc.publisherAmerican Chemical Societyen
dc.relation.urihttps://www.ncbi.nlm.nih.gov/pubmed/38393312en
dc.rightsCreative Commons Attribution 4.0 Internationalen
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/en
dc.titleSupramolecular Metal Halide Complexes for High-Temperature Non-linear Optical Switchesen
dc.title.serialJournal of the American Chemical Societyen
dc.typeArticle - Refereeden
dc.type.dcmitypeTexten
dc.type.otherArticleen
pubs.organisational-groupVirginia Techen
pubs.organisational-groupVirginia Tech/Scienceen
pubs.organisational-groupVirginia Tech/Science/Chemistryen
pubs.organisational-groupVirginia Tech/Faculty of Health Sciencesen
pubs.organisational-groupVirginia Tech/All T&R Facultyen
pubs.organisational-groupVirginia Tech/Science/COS T&R Facultyen
pubs.organisational-groupVirginia Tech/Report testen

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