Spontaneous and stimulated electron–photon interactions in nanoscale plasmonic near fields

Abstract The interplay between free electrons, light, and matter offers unique prospects for space, time, and energy resolved optical material characterization, structured light generation, and quantum information processing. Here, we study the nanoscale features of spontaneous and stimulated electr...

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Main Authors: Matthias Liebtrau, Murat Sivis, Armin Feist, Hugo Lourenço-Martins, Nicolas Pazos-Pérez, Ramon A. Alvarez-Puebla, F. Javier García de Abajo, Albert Polman, Claus Ropers
Format: Article
Language:English
Published: Nature Publishing Group 2021-04-01
Series:Light: Science & Applications
Online Access:https://doi.org/10.1038/s41377-021-00511-y
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author Matthias Liebtrau
Murat Sivis
Armin Feist
Hugo Lourenço-Martins
Nicolas Pazos-Pérez
Ramon A. Alvarez-Puebla
F. Javier García de Abajo
Albert Polman
Claus Ropers
author_facet Matthias Liebtrau
Murat Sivis
Armin Feist
Hugo Lourenço-Martins
Nicolas Pazos-Pérez
Ramon A. Alvarez-Puebla
F. Javier García de Abajo
Albert Polman
Claus Ropers
author_sort Matthias Liebtrau
collection DOAJ
description Abstract The interplay between free electrons, light, and matter offers unique prospects for space, time, and energy resolved optical material characterization, structured light generation, and quantum information processing. Here, we study the nanoscale features of spontaneous and stimulated electron–photon interactions mediated by localized surface plasmon resonances at the tips of a gold nanostar using electron energy-loss spectroscopy (EELS), cathodoluminescence spectroscopy (CL), and photon-induced near-field electron microscopy (PINEM). Supported by numerical electromagnetic boundary-element method (BEM) calculations, we show that the different coupling mechanisms probed by EELS, CL, and PINEM feature the same spatial dependence on the electric field distribution of the tip modes. However, the electron–photon interaction strength is found to vary with the incident electron velocity, as determined by the spatial Fourier transform of the electric near-field component parallel to the electron trajectory. For the tightly confined plasmonic tip resonances, our calculations suggest an optimum coupling velocity at electron energies as low as a few keV. Our results are discussed in the context of more complex geometries supporting multiple modes with spatial and spectral overlap. We provide fundamental insights into spontaneous and stimulated electron-light-matter interactions with key implications for research on (quantum) coherent optical phenomena at the nanoscale.
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spelling doaj.art-d23e10211a5a41be979658527d11c6272022-12-22T04:05:47ZengNature Publishing GroupLight: Science & Applications2047-75382021-04-0110111410.1038/s41377-021-00511-ySpontaneous and stimulated electron–photon interactions in nanoscale plasmonic near fieldsMatthias Liebtrau0Murat Sivis1Armin Feist2Hugo Lourenço-Martins3Nicolas Pazos-Pérez4Ramon A. Alvarez-Puebla5F. Javier García de Abajo6Albert Polman7Claus Ropers8Center for Nanophotonics, AMOLF4th Physical Institute–Solids and Nanostructures, University of Göttingen4th Physical Institute–Solids and Nanostructures, University of Göttingen4th Physical Institute–Solids and Nanostructures, University of GöttingenDepartment of Physical Chemistry and EMaS, Universitat Rovira i VirgiliDepartment of Physical Chemistry and EMaS, Universitat Rovira i VirgiliICREA–Institució Catalana de Recerca i Estudis AvançatsCenter for Nanophotonics, AMOLF4th Physical Institute–Solids and Nanostructures, University of GöttingenAbstract The interplay between free electrons, light, and matter offers unique prospects for space, time, and energy resolved optical material characterization, structured light generation, and quantum information processing. Here, we study the nanoscale features of spontaneous and stimulated electron–photon interactions mediated by localized surface plasmon resonances at the tips of a gold nanostar using electron energy-loss spectroscopy (EELS), cathodoluminescence spectroscopy (CL), and photon-induced near-field electron microscopy (PINEM). Supported by numerical electromagnetic boundary-element method (BEM) calculations, we show that the different coupling mechanisms probed by EELS, CL, and PINEM feature the same spatial dependence on the electric field distribution of the tip modes. However, the electron–photon interaction strength is found to vary with the incident electron velocity, as determined by the spatial Fourier transform of the electric near-field component parallel to the electron trajectory. For the tightly confined plasmonic tip resonances, our calculations suggest an optimum coupling velocity at electron energies as low as a few keV. Our results are discussed in the context of more complex geometries supporting multiple modes with spatial and spectral overlap. We provide fundamental insights into spontaneous and stimulated electron-light-matter interactions with key implications for research on (quantum) coherent optical phenomena at the nanoscale.https://doi.org/10.1038/s41377-021-00511-y
spellingShingle Matthias Liebtrau
Murat Sivis
Armin Feist
Hugo Lourenço-Martins
Nicolas Pazos-Pérez
Ramon A. Alvarez-Puebla
F. Javier García de Abajo
Albert Polman
Claus Ropers
Spontaneous and stimulated electron–photon interactions in nanoscale plasmonic near fields
Light: Science & Applications
title Spontaneous and stimulated electron–photon interactions in nanoscale plasmonic near fields
title_full Spontaneous and stimulated electron–photon interactions in nanoscale plasmonic near fields
title_fullStr Spontaneous and stimulated electron–photon interactions in nanoscale plasmonic near fields
title_full_unstemmed Spontaneous and stimulated electron–photon interactions in nanoscale plasmonic near fields
title_short Spontaneous and stimulated electron–photon interactions in nanoscale plasmonic near fields
title_sort spontaneous and stimulated electron photon interactions in nanoscale plasmonic near fields
url https://doi.org/10.1038/s41377-021-00511-y
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