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Unveiling Spatial and Temporal Dynamics of Plasmon-Enhanced Localized Fields in Metallic Nanoframes through Ultrafast Electron Microscopy

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    Unveiling Spatial and Temporal Dynamics of Plasmon-Enhanced Localized Fields in Metallic Nanoframes through Ultrafast Electron Microscopy
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    ACS Nano

    Cite this: ACS Nano 2024, 18, 41, 28258–28267
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    https://doi.org/10.1021/acsnano.4c08875
    Published October 1, 2024
    Copyright © 2024 American Chemical Society
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    Abstract

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    Plasmonic nanomaterials, particularly noble metal nanoframes (NFs), are important for applications such as catalysis, biosensing, and energy harvesting due to their ability to enhance localized electric fields and atomic efficiency via localized surface plasmon resonance (LSPR). Yet the fundamental structure–function relationships and plasmonic dynamics of the NFS are difficult to study experimentally and thus far rely predominately on computational methodologies, limiting their utilization. This study leverages the capabilities of ultrafast electron microscopy (UEM), specifically photon-induced near-field electron microscopy (PINEM), to probe the light-matter interactions within plasmonic NF structures. The effects of shape, size, and plasmonic coupling of Pt@Au core–shell NFs on spatial and temporal characteristics of plasmon-enhanced localized electric fields are explored. Importantly, time-resolved PINEM analysis reveals that the plasmonic fields around hexagonal NF prisms exhibit a spatially dependent excitation and decay rate, indicating a nuanced interplay between the spatial geometry of the NF and the temporal evolution of the localized electric field. These results and observations uncover nanophotonic energy transfer dynamics in NFs and highlight their potential for applications in biosensing and photocatalysis.

    Copyright © 2024 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsnano.4c08875.

    • SEM images of triangular prism nanoparticles and nanoframes; Extended extinction cross section of large hexagonal nanoframes; Polarization resolved UEM measurements of NFs; Demonstration of time-zero determination in UEM by time-resolved PINEM spectrum (PDF)

    • Supplementary Videos: Polarization dependent PINEM images of NFs; Supplementary Video: Time resolved PINEM images of NFs (ZIP)

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    ACS Nano

    Cite this: ACS Nano 2024, 18, 41, 28258–28267
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.4c08875
    Published October 1, 2024
    Copyright © 2024 American Chemical Society
    Request reuse permissions

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