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Link between Cathodoluminescence and Electron Energy Loss Spectroscopy and the Radiative and Full Electromagnetic Local Density of States

Losquin, Arthur LU and Kociak, Mathieu (2015) In ACS Photonics 2(11). p.1619-1627
Abstract
Electron energy loss spectroscopy (EELS) and cathodoluminescence (CL) have proved during the past few years to be tremendous tools to study surface plasmons in metallic nanoparticles, thanks to an extremely high spatial resolution combined with a broad spectral range. Despite their apparent close resemblance, qualitative differences between EELS and CL have been theoretically as well as experimentally pinpointed. We demonstrate that these differences are recovered when comparing the full electromagnetic local density of states (EMLDOS) and the radiative EMLDOS. Following the known relation established between EELS and the projection along the electron trajectory of the full EMLDOS, we introduce a formalism based on the Maxwell electric... (More)
Electron energy loss spectroscopy (EELS) and cathodoluminescence (CL) have proved during the past few years to be tremendous tools to study surface plasmons in metallic nanoparticles, thanks to an extremely high spatial resolution combined with a broad spectral range. Despite their apparent close resemblance, qualitative differences between EELS and CL have been theoretically as well as experimentally pinpointed. We demonstrate that these differences are recovered when comparing the full electromagnetic local density of states (EMLDOS) and the radiative EMLDOS. Following the known relation established between EELS and the projection along the electron trajectory of the full EMLDOS, we introduce a formalism based on the Maxwell electric Green tensor to draw a link between CL and the projection along the electron trajectory of the radiative EMLDOS. We discuss in simple terms the differences between EELS (projected full EMLDOS) and CL (projected radiative EMLDOS) through modal decompositions obtained in the quasistatic approximation. Contrary to EELS, CL probes only the radiative modes. Furthermore, CL resonant line shapes may be shifted and asymmetric compared to EELS. The CL asymmetry is due to interferences in the far-field radiation from spectrally and spatially overlapping modes. Our analytical expressions are illustrated through boundary element method numerical simulations. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
nanooptics, plasmonics, electron energy loss spectroscopy, cathodoluminescence, electromagnetic local density of states
in
ACS Photonics
volume
2
issue
11
pages
1619 - 1627
publisher
The American Chemical Society
external identifiers
  • wos:000365148400015
  • scopus:84947968282
ISSN
2330-4022
DOI
10.1021/acsphotonics.5b00416
language
English
LU publication?
yes
id
ff8280ab-b826-4f53-89eb-10b4d9162295 (old id 8539575)
date added to LUP
2016-01-20 12:57:08
date last changed
2017-07-09 04:02:45
@article{ff8280ab-b826-4f53-89eb-10b4d9162295,
  abstract     = {Electron energy loss spectroscopy (EELS) and cathodoluminescence (CL) have proved during the past few years to be tremendous tools to study surface plasmons in metallic nanoparticles, thanks to an extremely high spatial resolution combined with a broad spectral range. Despite their apparent close resemblance, qualitative differences between EELS and CL have been theoretically as well as experimentally pinpointed. We demonstrate that these differences are recovered when comparing the full electromagnetic local density of states (EMLDOS) and the radiative EMLDOS. Following the known relation established between EELS and the projection along the electron trajectory of the full EMLDOS, we introduce a formalism based on the Maxwell electric Green tensor to draw a link between CL and the projection along the electron trajectory of the radiative EMLDOS. We discuss in simple terms the differences between EELS (projected full EMLDOS) and CL (projected radiative EMLDOS) through modal decompositions obtained in the quasistatic approximation. Contrary to EELS, CL probes only the radiative modes. Furthermore, CL resonant line shapes may be shifted and asymmetric compared to EELS. The CL asymmetry is due to interferences in the far-field radiation from spectrally and spatially overlapping modes. Our analytical expressions are illustrated through boundary element method numerical simulations.},
  author       = {Losquin, Arthur and Kociak, Mathieu},
  issn         = {2330-4022},
  keyword      = {nanooptics,plasmonics,electron energy loss spectroscopy,cathodoluminescence,electromagnetic local density of states},
  language     = {eng},
  number       = {11},
  pages        = {1619--1627},
  publisher    = {The American Chemical Society},
  series       = {ACS Photonics},
  title        = {Link between Cathodoluminescence and Electron Energy Loss Spectroscopy and the Radiative and Full Electromagnetic Local Density of States},
  url          = {http://dx.doi.org/10.1021/acsphotonics.5b00416},
  volume       = {2},
  year         = {2015},
}