Continuous Wave Resonant Photon Stimulated Electron Energy-Gain and Electron Energy-Loss Spectroscopy of Individual Plasmonic Nanoparticles

Liu, Chenze; Wu, Yueying; Hu, Zhongwei; Busche, Jacob A.; Beutler, Elliot K.; Montoni, Nicholas P.; Moore, Thomas M.; Magel, Gregory A.; Camden, Jon P.; Masiello, David J.; Duscher, Gerd; Rack, Philip D.

doi:10.1021/acsphotonics.9b00830

Continuous Wave Resonant Photon Stimulated Electron Energy-Gain and Electron Energy-Loss Spectroscopy of Individual Plasmonic Nanoparticles

Journal Article · Wed Aug 28 00:00:00 EDT 2019 · ACS Photonics

DOI:https://doi.org/10.1021/acsphotonics.9b00830· OSTI ID:1597429

^[1]; ^[2]; ^[3]; ^[3]; Beutler, Elliot K. ^[3]; Montoni, Nicholas P. ^[3]; Moore, Thomas M. ^[4]; Magel, Gregory A. ^[5]; ^[6]; ^[3]; Duscher, Gerd ^[7]; ^[8]

Univ. of Tennessee, Knoxville, TN (United States); University of Washington
Univ. of Tennessee, Knoxville, TN (United States); Univ. of Notre Dame, IN (United States)
Univ. of Washington, Seattle, WA (United States)
Waviks Inc., Dallas, TX (United States)
Waviks Inc., Dallas, TX (United States)
Univ. of Notre Dame, IN (United States)
Univ. of Tennessee, Knoxville, TN (United States)
Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

The unique optical properties of surface plasmon resonances in nanostructured materials have attracted considerable attention, broadly impacting both fundamental research and applied technologies ranging from sensing and optoelectronics to quantum computing. Electron energy-loss spectroscopy (EELS) in the transmission electron microscope has revealed valuable information about the full plasmonic spectrum of these materials with nanoscale spatial resolution. Here, in this study, we report a novel approach for experimentally accessing the photon-stimulated electron energy-gain and stimulated electron energy-loss responses of individual plasmonic nanoparticles via the simultaneous irradiation of a continuous wave laser and continuous current, monochromated electron probe. Stimulated gain and loss probabilities are equivalent and increase linearly in the low-irradiance range of 0.5 × 10⁸ to 4 × 10⁸ W/m², above which excessive heating reduces the observed probabilities; importantly in our low-irradiance regime, the photon energy must be tuned in resonance with the plasmon energy for the stimulated gain and loss peaks to emerge. Theoretical modeling based on Fermi’s golden rule elucidates how the plasmon resonantly and coherently shuttles energy quanta between the electron probe and the radiation field and vice versa in stimulated electron energy-loss and -gain events. This study opens a fundamentally new approach to explore the quantum physics of excited-state plasmon resonances that does not rely on high-intensity laser pulses or any modification to the EELS detector.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of Notre Dame, IN (United States); Univ. of Washington, Seattle, WA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC05-00OR22725; SC0018040; SC0018169

OSTI ID:: 1597429

Alternate ID(s):: OSTI ID: 1846553
OSTI ID: 1907179

Journal Information:: ACS Photonics, Journal Name: ACS Photonics Journal Issue: 10 Vol. 6; ISSN 2330-4022

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Continuous Wave Resonant Photon Stimulated Electron Energy-Gain and Electron Energy-Loss Spectroscopy of Individual Plasmonic Nanoparticles

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