Snapshot Hyperspectral Imaging (SHI) for Revealing Irreversible and Heterogeneous Plasmonic Processes

Abstract

Plasmon-mediated processes provide unique opportunities for selective photocatalysis, photovoltaics, and electrochemistry. Determining the influence of particle heterogeneity is an unsolved problem because often such processes introduce irreversible changes to the nanocatalysts and/or their surroundings. The challenge lies in monitoring heterogeneous nonequilibrium dynamics via the slow, serial methods that are intrinsic to almost all spectral acquisition methods with suitable spatial and/or spectral resolution. Here, we present a new metrology, snapshot hyperspectral imaging (SHI), that facilitates in situ readout of the tube lens image and first-order diffraction image of the dark-field scattering from many individual plasmonic nanoparticles to extract their respective spectra simultaneously. Evanescent wave excitation with a supercontinuum laser enabled signal-to-noise ratios greater than 100 with a time resolution of only 1 ms. Throughput of ∼100 simultaneous spectra was achieved with a highly ordered nanoparticle array, yielding a spectral resolution of 0.21 nm/pixel. Additionally, an alternative dark-field excitation geometry utilized a combination of a supercontinuum laser and a reflecting objective for polarization-controlled SHI. Using a simplified version of SHI, we temporally resolve on the millisecond time scale the heterogeneous kinetics of an electrochemical surface redox reaction for many individual gold nanoparticles simultaneously.

Description
Advisor
Degree
Type
Journal article
Keywords
Citation

Kirchner, Silke R., Smith, Kyle W., Hoener, Benjamin S., et al.. "Snapshot Hyperspectral Imaging (SHI) for Revealing Irreversible and Heterogeneous Plasmonic Processes." The Journal of Physical Chemistry C, 122, no. 12 (2018) American Chemical Society: 6865-6875. https://doi.org/10.1021/acs.jpcc.8b01398.

Has part(s)
Forms part of
Rights
This is an open access article published under an ACS AuthorChoiceᅠLicense, which permits copying and redistribution of the article or any adaptations for non-commercial purposes.
Citable link to this page