Active control of strong plasmon-exciton coupling in biomimetic pigment-polymer antenna complexes grown by surface-initiated polymerisation from gold nanostructures

LISHCHUK, A., CSÁNYI, E., DARROCH, B., WILSON, C., NABOK, Aleksey and LEGGETT, G.J. (2022). Active control of strong plasmon-exciton coupling in biomimetic pigment-polymer antenna complexes grown by surface-initiated polymerisation from gold nanostructures. Chemical Science, 13 (8), 2405-2417.

[img]
Preview
PDF
Nabok-ActiveControlStrong(VoR).pdf - Published Version
Creative Commons Attribution.

Download (1MB) | Preview
Official URL: https://pubs.rsc.org/en/content/articlelanding/202...
Open Access URL: https://pubs.rsc.org/en/content/articlepdf/2022/sc... (Published version)
Link to published version:: https://doi.org/10.1039/d1sc05842h
Related URLs:

    Abstract

    Plexcitonic antenna complexes, inspired by photosynthetic light-harvesting complexes, are formed by attachment of chlorophylls (Chl) to poly(cysteine methacrylate) (PCysMA) scaffolds grown by atom-transfer radical polymerisation from gold nanostructure arrays. In these pigment-polymer antenna complexes, localised surface plasmon resonances on gold nanostructures are strongly coupled to Chl excitons, yielding hybrid light-matter states (plexcitons) that are manifested in splitting of the plasmon band. Modelling of the extinction spectra of these systems using a simple coupled oscillator model indicates that their coupling energies are up to twice as large as those measured for LHCs from plants and bacteria. Coupling energies are correlated with the exciton density in the grafted polymer layer, consistent with the collective nature of strong plasmon-exciton coupling. Steric hindrance in fully-dense PCysMA brushes limits binding of bulky chlorophylls, but the chlorophyll concentration can be increased to ∼2 M, exceeding that in biological light-harvesting complexes, by controlling the grafting density and polymerisation time. Moreover, synthetic plexcitonic antenna complexes display pH- and temperature-responsiveness, facilitating active control of plasmon-exciton coupling. Because of the wide range of compatible polymer chemistries and the mild reaction conditions, plexcitonic antenna complexes may offer a versatile route to programmable molecular photonic materials. This journal is

    Item Type: Article
    Uncontrolled Keywords: 03 Chemical Sciences
    Identification Number: https://doi.org/10.1039/d1sc05842h
    Page Range: 2405-2417
    SWORD Depositor: Symplectic Elements
    Depositing User: Symplectic Elements
    Date Deposited: 17 Mar 2022 14:53
    Last Modified: 17 Mar 2022 15:00
    URI: http://shura.shu.ac.uk/id/eprint/29953

    Actions (login required)

    View Item View Item

    Downloads

    Downloads per month over past year

    View more statistics