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

Abstract

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 physicsmore » of excited-state plasmon resonances that does not rely on high-intensity laser pulses or any modification to the EELS detector.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [3];  [3];  [3];  [4];  [5]; ORCiD logo [6]; ORCiD logo [3];  [1]; ORCiD logo [7]
+ Show Author Affiliations
  1. Univ. of Tennessee, Knoxville, TN (United States)
  2. Univ. of Tennessee, Knoxville, TN (United States); Univ. of Notre Dame, IN (United States)
  3. Univ. of Washington, Seattle, WA (United States)
  4. Waviks Inc., Dallas, TX (United States)
  5. Waviks Inc., Dallas, TX (United States)
  6. Univ. of Notre Dame, IN (United States)
  7. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Univ. of Washington, Seattle, WA (United States); Univ. of Notre Dame, IN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1597429
Alternate Identifier(s):
OSTI ID: 1846553; OSTI ID: 1907179
Grant/Contract Number:  
SC0018040; SC0018169; AC05-00OR22725; DMR-1709275; 1709601; SBIR-1721719
Resource Type:
Accepted Manuscript
Journal Name:
ACS Photonics
Additional Journal Information:
Journal Volume: 6; Journal Issue: 10; Journal ID: ISSN 2330-4022
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; plasmon resonance; electron energy loss (EEL); electron energy gain (EEG); (scanning) transmission electron microscope ((S)TEM); laser; electron energy loss spectroscopy; electrical energy; plasmons; mathematical methods; lasers

Citation Formats

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, and Rack, Philip D. Continuous Wave Resonant Photon Stimulated Electron Energy-Gain and Electron Energy-Loss Spectroscopy of Individual Plasmonic Nanoparticles. United States: N. p., 2019. Web. doi:10.1021/acsphotonics.9b00830.
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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. Continuous Wave Resonant Photon Stimulated Electron Energy-Gain and Electron Energy-Loss Spectroscopy of Individual Plasmonic Nanoparticles. United States. https://doi.org/10.1021/acsphotonics.9b00830
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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, and Rack, Philip D. Wed . "Continuous Wave Resonant Photon Stimulated Electron Energy-Gain and Electron Energy-Loss Spectroscopy of Individual Plasmonic Nanoparticles". United States. https://doi.org/10.1021/acsphotonics.9b00830. https://www.osti.gov/servlets/purl/1597429.
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@article{osti_1597429,
title = {Continuous Wave Resonant Photon Stimulated Electron Energy-Gain and Electron Energy-Loss Spectroscopy of Individual Plasmonic Nanoparticles},
author = {Liu, Chenze and Wu, Yueying and Hu, Zhongwei and Busche, Jacob A. and Beutler, Elliot K. and Montoni, Nicholas P. and Moore, Thomas M. and Magel, Gregory A. and Camden, Jon P. and Masiello, David J. and Duscher, Gerd and Rack, Philip D.},
abstractNote = {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.},
doi = {10.1021/acsphotonics.9b00830},
journal = {ACS Photonics},
number = 10,
volume = 6,
place = {United States},
year = {Wed Aug 28 00:00:00 EDT 2019},
month = {Wed Aug 28 00:00:00 EDT 2019}
}
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https://doi.org/10.1021/acsphotonics.9b00830
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