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Chiral Photomelting of DNA-Nanocrystal Assemblies Utilizing Plasmonic Photoheating

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    Chiral Photomelting of DNA-Nanocrystal Assemblies Utilizing Plasmonic Photoheating
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    Nano Letters

    Cite this: Nano Lett. 2021, 21, 17, 7298–7308
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    https://doi.org/10.1021/acs.nanolett.1c02479
    Published August 24, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    Chiral plasmonic nanostructures exhibit anomalously strong chiroptical signals and offer the possibility to realize asymmetric photophysical and photochemical processes controlled by circularly polarized light. Here, we use a chiral DNA-assembled nanorod pair as a model system for chiral plasmonic photomelting. We show that both the enantiomeric excess and consequent circular dichroism can be controlled with chiral light. The nonlinear chiroptical response of our plasmonic system results from the chiral photothermal effect leading to selective melting of the DNA linker strands. Our study describes both the single-complex and collective heating regimes, which should be treated with different models. The chiral asymmetry factors of the calculated photothermal and photomelting effects exceed the values typical for the chiral molecular photochemistry at least 10-fold. Our proposed mechanism can be used to develop chiral photoresponsive systems controllable with circularly polarized light.

    Copyright © 2021 American Chemical Society

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    • Model for the collective and single-particle heating regimes; additional numerical data for the chiral plasmonic complexes (PDF)

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    Cited By

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    This article is cited by 24 publications.

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    Nano Letters

    Cite this: Nano Lett. 2021, 21, 17, 7298–7308
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.nanolett.1c02479
    Published August 24, 2021
    Copyright © 2021 American Chemical Society
    Request reuse permissions

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