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

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  • Calvin Boerigter

    (University of Michigan)

  • Robert Campana

    (University of Michigan)

  • Matthew Morabito

    (University of Michigan)

  • Suljo Linic

    (University of Michigan)

Abstract

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. 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.

Suggested Citation

  • Calvin Boerigter & Robert Campana & Matthew Morabito & Suljo Linic, 2016. "Evidence and implications of direct charge excitation as the dominant mechanism in plasmon-mediated photocatalysis," Nature Communications, Nature, vol. 7(1), pages 1-9, April.
    • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms10545
    DOI: 10.1038/ncomms10545
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    Cited by:

    1. Qi Zhang & Wei Li & Ruixuan Zhao & Peizhe Tang & Jie Zhao & Guorong Wu & Xin Chen & Mingjun Hu & Kaijun Yuan & Jiebo Li & Xueming Yang, 2024. "Real-time observation of two distinctive non-thermalized hot electron dynamics at MXene/molecule interfaces," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Ibrahim Deneme & Gorkem Liman & Ayse Can & Gokhan Demirel & Hakan Usta, 2021. "Enabling three-dimensional porous architectures via carbonyl functionalization and molecular-specific organic-SERS platforms," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    3. Canyu Hu & Xing Chen & Jingxiang Low & Yaw-Wen Yang & Hao Li & Di Wu & Shuangming Chen & Jianbo Jin & He Li & Huanxin Ju & Chia-Hsin Wang & Zhou Lu & Ran Long & Li Song & Yujie Xiong, 2023. "Near-infrared-featured broadband CO2 reduction with water to hydrocarbons by surface plasmon," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    4. Yicui Kang & Simão M. João & Rui Lin & Kang Liu & Li Zhu & Junwei Fu & Weng-Chon (Max) Cheong & Seunghoon Lee & Kilian Frank & Bert Nickel & Min Liu & Johannes Lischner & Emiliano Cortés, 2024. "Effect of crystal facets in plasmonic catalysis," Nature Communications, Nature, vol. 15(1), pages 1-13, December.

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