Evidence and implications of direct charge excitation as the dominant mechanism in plasmon-mediated photocatalysis

Boerigter, Calvin; Campana, Robert; Morabito, Matthew; Linic, Suljo

doi:10.1038/ncomms10545

Evidence and implications of direct charge excitation as the dominant mechanism in plasmon-mediated photocatalysis

Journal Article · Thu Jan 28 00:00:00 EST 2016 · Nature Communications

DOI:https://doi.org/10.1038/ncomms10545· OSTI ID:1242978

Boerigter, Calvin ^[1]; Campana, Robert ^[2]; Morabito, Matthew ^[2]; Linic, Suljo ^[2]

Univ. of Michigan, Ann Arbor, MI (United States); University of Michigan
Univ. of Michigan, Ann Arbor, MI (United States)

Plasmonic metal nanoparticles enhance chemical reactions on their surface when illuminated with light of particular frequencies. It has been shown that these processes are driven by excitation of localized surface plasmon resonance (LSPR). The interaction of LSPR with adsorbate orbitals can lead to the injection of energized charge carriers into the adsorbate, which can result in chemical transformations. The mechanism of the charge injection process (and role of LSPR) is not well understood. Here we shed light on the specifics of this mechanism by coupling optical characterization methods, mainly wavelength-dependent Stokes and anti-Stokes SERS, with kinetic analysis of photocatalytic reactions in an Ag nanocube–methylene blue plasmonic system. We propose that localized LSPR-induced electric fields result in a direct charge transfer within the molecule–adsorbate system. Lastly, these observations provide a foundation for the development of plasmonic catalysts that can selectively activate targeted chemical bonds, since the mechanism allows for tuning plasmonic nanomaterials in such a way that illumination can selectively enhance desired chemical pathways.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Michigan, Ann Arbor, MI (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: FG02-05ER15686

OSTI ID:: 1242978

Journal Information:: Nature Communications, Journal Name: Nature Communications Vol. 7; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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