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    Nanoscale Silicon Oxide Reduces Electron Transfer Kinetics of Surface-Bound Ferrocene Monolayers on Silicon

    93730.pdf (1.342Mb)
    Access Status
    Open access
    Authors
    Li, Tiexin
    Dief, Essam
    Lyu, Xin
    Rahpeima, Soraya
    Ciampi, Simone
    Darwish, Nadim
    Date
    2021
    Type
    Journal Article
    
    Metadata
    Show full item record
    Citation
    Li, T. and Dief, E.M. and Lyu, X. and Rahpeima, S. and Ciampi, S. and Darwish, N. 2021. Nanoscale Silicon Oxide Reduces Electron Transfer Kinetics of Surface-Bound Ferrocene Monolayers on Silicon. Journal of Physical Chemistry C. 125 (50): pp. 27763-27770.
    Source Title
    Journal of Physical Chemistry C
    DOI
    10.1021/acs.jpcc.1c07788
    ISSN
    1932-7447
    Faculty
    Faculty of Science and Engineering
    School
    School of Molecular and Life Sciences (MLS)
    Funding and Sponsorship
    http://purl.org/au-research/grants/arc/DP190100735
    Remarks

    This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Physical Chemistry C, copyright © American Chemical Society, after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.jpcc.1c07788.

    URI
    http://hdl.handle.net/20.500.11937/93926
    Collection
    • Curtin Research Publications
    Abstract

    Functionalizing Si with self-assembled monolayers (SAMs) paves the way for integrating the semiconducting properties of Si with the diverse properties of organic molecules. Highly packed SAMs such as those formed from alkyl chains protect Si from reoxidation in an ambient environment. Such monolayers have been largely considered oxide-free, but the effect of nanoscale reoxidation on the electrochemical kinetics of Si-based SAMs remains unknown. Here, we systematically study the effect of the oxide growth on the electrochemical charge-transfer kinetics of ferrocene-terminated SAMs on Si by exposing the surfaces to ambient conditions for controlled periods of time. X-ray photoelectron spectroscopy and atomic force microscopy revealed a gradual growth of silicon oxide (SiOx) on the surfaces over time. The oxide growth is accompanied by a decrease in the ferrocene surface coverage and a concomitant decrease in the electron transfer rate constant (ket) measured by electrochemical impedance spectroscopy. The drop in ket is attributed to a greater spacing between the ferrocene moieties induced by the surface oxide, which in turn blocks lateral electron transfer between neighboring ferrocene moieties. These findings explain the highly scattered literature data on electron transfer kinetics for monolayers on Si and have implications for the proper design of Si-based molecular electronic devices.

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