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    Direct Visualization of a Gold Nanoparticle Electron Trapping Effect

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    Type
    Article
    Authors
    Williams, Oscar Bentley Jerdmyr
    Katsiev, Khabiboulakh
    Baek, Byeongjin cc
    Harrison, George
    Thornton, G. cc
    Idriss, Hicham cc
    KAUST Department
    KAUST Solar Center (KSC)
    Physical Science and Engineering (PSE) Division
    Surface Science and Advanced Characterisation, SABIC-CRD at King Abdullah University for Science and Technology (KAUST), Thuwal, 23955, Saudi Arabia
    Date
    2022-01-05
    Embargo End Date
    2023-01-05
    Submitted Date
    2021-11-18
    Permanent link to this record
    http://hdl.handle.net/10754/675023
    
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    Abstract
    A new atomic-scale anisotropy in the photoreaction of surface carboxylates on rutile TiO<sub>2</sub>(110) induced by gold clusters is found. STM and DFT+U are used to study this phenomenon by monitoring the photoreaction of a prototype hole-scavenger molecule, benzoic acid, over stoichiometric (s) s-TiO<sub>2</sub>, Au<sub>9</sub>/s-TiO<sub>2</sub>, and reduced (r) Au<sub>9</sub>/r-TiO<sub>2</sub>. STM results show that benzoic acid adsorption displaces a large fraction of Au clusters from the terraces toward their edges. DFT calculations explain that Au<sub>9</sub> clusters on stoichiometric TiO<sub>2</sub> are distorted by benzoic acid adsorption. The influence of sub-monolayers of Au on the UV/visible photoreaction of benzoic acid was explored at room temperature, with adsorbate depletion taken as a measure of activity. The empty sites, observed upon photoexcitation, occurred in elongated chains (2 to 6 molecules long) in the [11̅0] and [001] directions. A roughly 3-fold higher depletion rate is observed in the [001] direction. This is linked to the anisotropic conduction of excited electrons along [001], with subsequent trapping by Au clusters leaving a higher concentration of holes and thus an increased decomposition rate. To our knowledge this is the first time that atomic-scale directionality of a chemical reaction is reported upon photoexcitation of the semiconductor.
    Citation
    Williams, O. B. J., Katsiev, K., Baek, B., Harrison, G., Thornton, G., & Idriss, H. (2022). Direct Visualization of a Gold Nanoparticle Electron Trapping Effect. Journal of the American Chemical Society. doi:10.1021/jacs.1c12197
    Sponsors
    This work was supported by the European Research Council Advanced Grant ENERGYSURF and EPSRC (U.K.) (EP/L015277/1).
    Publisher
    American Chemical Society (ACS)
    Journal
    Journal of the American Chemical Society
    DOI
    10.1021/jacs.1c12197
    PubMed ID
    34985273
    Additional Links
    https://pubs.acs.org/doi/10.1021/jacs.1c12197
    https://discovery.ucl.ac.uk/10141905/1/Thornton_Williams%20et%20al%20revised.pdf
    ae974a485f413a2113503eed53cd6c53
    10.1021/jacs.1c12197
    Scopus Count
    Collections
    Articles; Physical Science and Engineering (PSE) Division; KAUST Solar Center (KSC)

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