Cathodoluminescence excitation spectroscopy: Nanoscale imaging of excitation pathways

Nadezda Varkentina; Yves Auad; Steffi Y. Woo; Alberto Zobelli; Laura Bocher; Jean Denis Blazit; Xiaoyan Li; Marcel Tencé; Kenji Watanabe; Takashi Taniguchi; Odile Stéphan; Mathieu Kociak; Luiz H.G. Tizei

doi:10.1126/sciadv.abq4947

Cathodoluminescence excitation spectroscopy: Nanoscale imaging of excitation pathways

Nadezda Varkentina, Yves Auad, Steffi Y. Woo, Alberto Zobelli, Laura Bocher, Jean Denis Blazit, Xiaoyan Li, Marcel Tencé, Kenji Watanabe, Takashi Taniguchi, Odile Stéphan, Mathieu Kociak, Luiz H.G. Tizei

Research output: Contribution to journal › Article › peer-review

31 Scopus citations

Abstract

Following optical excitations’ life span from creation to decay into photons is crucial in understanding materials photophysics. Macroscopically, this is studied using optical techniques, such as photoluminescence excitation spectroscopy. However, excitation and emission pathways can vary at nanometer scales, preventing direct access, as no characterization technique has the relevant spatial, spectral, and time resolution. Here, using combined electron spectroscopies, we explore excitations’ creation and decay in two representative optical materials: plasmonic nanoparticles and luminescent two-dimensional layers. The analysis of the energy lost by an exciting electron that is coincident in time with a visible-ultraviolet photon unveils the decay pathways from excitation toward light emission. This is demonstrated for phase-locked (coherent) interactions (localized surface plasmons) and non–phase-locked ones (point defect excited states). The developed cathodoluminescence excitation spectroscopy images energy transfer pathways at the nanometer scale, widening the available toolset to explore nanoscale materials.

Original language	English
Article number	eabq4947
Journal	Science Advances
Volume	8
Issue number	40
DOIs	https://doi.org/10.1126/sciadv.abq4947
State	Published - Oct 2022
Externally published	Yes

Funding

We thank ASI for extensive discussion during the Timepix3 CheeTah implementation for EELS and coincidence experiments. This project has been funded in part by the National Agency for Research under the program of future investment TEMPOS-CHROMATEM (reference no. ANR-10-EQPX-50), the JCJC grant SpinE (reference no. ANR-20-CE42-0020), the BONASPES project (ANR-19-CE30-0007) and the JCJC IMPULSE (reference no. ANR-19-CE42-0001), and by the European Union’s Horizon 2020 research and innovation programme under grant agreement nos. 823717 (ESTEEM3) and 101017720 (EBEAM). K.W. and T.T. acknowledge support from the Elemental Strategy Initiative conducted by the MEXT, Japan (grant no. JPMXP0112101001) and JSPS KAKENHI (grant nos. 19H05790, 20H00354, and 21H05233).

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@article{380db1cee23c46ddb772441263a90c79,

title = "Cathodoluminescence excitation spectroscopy: Nanoscale imaging of excitation pathways",

abstract = "Following optical excitations{\textquoteright} life span from creation to decay into photons is crucial in understanding materials photophysics. Macroscopically, this is studied using optical techniques, such as photoluminescence excitation spectroscopy. However, excitation and emission pathways can vary at nanometer scales, preventing direct access, as no characterization technique has the relevant spatial, spectral, and time resolution. Here, using combined electron spectroscopies, we explore excitations{\textquoteright} creation and decay in two representative optical materials: plasmonic nanoparticles and luminescent two-dimensional layers. The analysis of the energy lost by an exciting electron that is coincident in time with a visible-ultraviolet photon unveils the decay pathways from excitation toward light emission. This is demonstrated for phase-locked (coherent) interactions (localized surface plasmons) and non–phase-locked ones (point defect excited states). The developed cathodoluminescence excitation spectroscopy images energy transfer pathways at the nanometer scale, widening the available toolset to explore nanoscale materials.",

author = "Nadezda Varkentina and Yves Auad and Woo, {Steffi Y.} and Alberto Zobelli and Laura Bocher and Blazit, {Jean Denis} and Xiaoyan Li and Marcel Tenc{\'e} and Kenji Watanabe and Takashi Taniguchi and Odile St{\'e}phan and Mathieu Kociak and Tizei, {Luiz H.G.}",

note = "Publisher Copyright: Copyright {\textcopyright} 2022 The Authors, some rights reserved.",

year = "2022",

month = oct,

doi = "10.1126/sciadv.abq4947",

language = "English",

volume = "8",

journal = "Science Advances",

issn = "2375-2548",

publisher = "American Association for the Advancement of Science",

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T1 - Cathodoluminescence excitation spectroscopy

T2 - Nanoscale imaging of excitation pathways

AU - Varkentina, Nadezda

AU - Auad, Yves

AU - Woo, Steffi Y.

AU - Zobelli, Alberto

AU - Bocher, Laura

AU - Blazit, Jean Denis

AU - Li, Xiaoyan

AU - Tencé, Marcel

AU - Watanabe, Kenji

AU - Taniguchi, Takashi

AU - Stéphan, Odile

AU - Kociak, Mathieu

AU - Tizei, Luiz H.G.

PY - 2022/10

Y1 - 2022/10

N2 - Following optical excitations’ life span from creation to decay into photons is crucial in understanding materials photophysics. Macroscopically, this is studied using optical techniques, such as photoluminescence excitation spectroscopy. However, excitation and emission pathways can vary at nanometer scales, preventing direct access, as no characterization technique has the relevant spatial, spectral, and time resolution. Here, using combined electron spectroscopies, we explore excitations’ creation and decay in two representative optical materials: plasmonic nanoparticles and luminescent two-dimensional layers. The analysis of the energy lost by an exciting electron that is coincident in time with a visible-ultraviolet photon unveils the decay pathways from excitation toward light emission. This is demonstrated for phase-locked (coherent) interactions (localized surface plasmons) and non–phase-locked ones (point defect excited states). The developed cathodoluminescence excitation spectroscopy images energy transfer pathways at the nanometer scale, widening the available toolset to explore nanoscale materials.

AB - Following optical excitations’ life span from creation to decay into photons is crucial in understanding materials photophysics. Macroscopically, this is studied using optical techniques, such as photoluminescence excitation spectroscopy. However, excitation and emission pathways can vary at nanometer scales, preventing direct access, as no characterization technique has the relevant spatial, spectral, and time resolution. Here, using combined electron spectroscopies, we explore excitations’ creation and decay in two representative optical materials: plasmonic nanoparticles and luminescent two-dimensional layers. The analysis of the energy lost by an exciting electron that is coincident in time with a visible-ultraviolet photon unveils the decay pathways from excitation toward light emission. This is demonstrated for phase-locked (coherent) interactions (localized surface plasmons) and non–phase-locked ones (point defect excited states). The developed cathodoluminescence excitation spectroscopy images energy transfer pathways at the nanometer scale, widening the available toolset to explore nanoscale materials.

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JO - Science Advances

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Cathodoluminescence excitation spectroscopy: Nanoscale imaging of excitation pathways

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