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Coherent Excitation and Control of Plasmons on Gold Using Two-Dimensional Transition Metal Dichalcogenides

Vogelsang, Jan LU ; Wittenbecher, Lukas LU ; Pan, Deng ; Sun, Jiawei ; Mikaelsson, Sara LU ; Arnold, Cord L. LU ; Lhuillier, Anne LU orcid ; Xu, Hongxing LU and Mikkelsen, Anders LU (2021) In ACS Photonics 8(6). p.1607-1615
Abstract

The hybrid combination of two-dimensional (2D) transition metal dichalcogenides (TMDs) and plasmonic materials open up novel means of (ultrafast) optoelectronic applications and manipulation of nanoscale light-matter interaction. However, control of the plasmonic excitations by TMDs themselves has not been investigated. Here, we show that the ultrathin 2D WSe2 crystallites permit nanoscale spatially controlled coherent excitation of surface plasmon polaritons (SPPs) on smooth Au films. The resulting complex plasmonic interference patterns are recorded with nanoscale resolution in a photoemission electron microscope. Modeling shows good agreement with experiments and further indicates how SPPs can be tailored with high spatiotemporal... (More)

The hybrid combination of two-dimensional (2D) transition metal dichalcogenides (TMDs) and plasmonic materials open up novel means of (ultrafast) optoelectronic applications and manipulation of nanoscale light-matter interaction. However, control of the plasmonic excitations by TMDs themselves has not been investigated. Here, we show that the ultrathin 2D WSe2 crystallites permit nanoscale spatially controlled coherent excitation of surface plasmon polaritons (SPPs) on smooth Au films. The resulting complex plasmonic interference patterns are recorded with nanoscale resolution in a photoemission electron microscope. Modeling shows good agreement with experiments and further indicates how SPPs can be tailored with high spatiotemporal precision using the shape of the 2D TMDs with thicknesses down to single molecular layers. We demonstrate the use of WSe2 nanocrystals as 2D optical elements for exploring the ultrafast dynamics of SPPs. Using few-femtosecond laser pulse pairs we excite an SPP at the boundary of a WSe2 crystal and then have a WSe2 monolayer wedge act as a delay line inducing a spatially varying phase difference down to the attosecond time range. The observed effects are a natural yet unexplored consequence of high dielectric functional values of TMDs in the visible range that should be considered when designing metal-TMD hybrid devices. As the 2D TMD crystals are stable in air, can be defect free, can be synthesized in many shapes, and are reliably positioned on metal surfaces, using them to excite and steer SPPs adds an interesting alternative in designing hybrid structures for plasmonic control.

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author
; ; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
metal semiconductor hybrid systems, surface plasmon polaritons, time-resolved photoemission electron microscopy, transition metal dichalcogenides, ultrafast plasmonics
in
ACS Photonics
volume
8
issue
6
pages
9 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • scopus:85108440847
  • pmid:34307766
ISSN
2330-4022
DOI
10.1021/acsphotonics.0c01795
language
English
LU publication?
yes
id
d48674fa-4395-456b-ae2d-f61809dc7780
date added to LUP
2021-12-27 13:13:15
date last changed
2024-07-14 01:48:30
@article{d48674fa-4395-456b-ae2d-f61809dc7780,
  abstract     = {{<p>The hybrid combination of two-dimensional (2D) transition metal dichalcogenides (TMDs) and plasmonic materials open up novel means of (ultrafast) optoelectronic applications and manipulation of nanoscale light-matter interaction. However, control of the plasmonic excitations by TMDs themselves has not been investigated. Here, we show that the ultrathin 2D WSe2 crystallites permit nanoscale spatially controlled coherent excitation of surface plasmon polaritons (SPPs) on smooth Au films. The resulting complex plasmonic interference patterns are recorded with nanoscale resolution in a photoemission electron microscope. Modeling shows good agreement with experiments and further indicates how SPPs can be tailored with high spatiotemporal precision using the shape of the 2D TMDs with thicknesses down to single molecular layers. We demonstrate the use of WSe2 nanocrystals as 2D optical elements for exploring the ultrafast dynamics of SPPs. Using few-femtosecond laser pulse pairs we excite an SPP at the boundary of a WSe2 crystal and then have a WSe2 monolayer wedge act as a delay line inducing a spatially varying phase difference down to the attosecond time range. The observed effects are a natural yet unexplored consequence of high dielectric functional values of TMDs in the visible range that should be considered when designing metal-TMD hybrid devices. As the 2D TMD crystals are stable in air, can be defect free, can be synthesized in many shapes, and are reliably positioned on metal surfaces, using them to excite and steer SPPs adds an interesting alternative in designing hybrid structures for plasmonic control. </p>}},
  author       = {{Vogelsang, Jan and Wittenbecher, Lukas and Pan, Deng and Sun, Jiawei and Mikaelsson, Sara and Arnold, Cord L. and Lhuillier, Anne and Xu, Hongxing and Mikkelsen, Anders}},
  issn         = {{2330-4022}},
  keywords     = {{metal semiconductor hybrid systems; surface plasmon polaritons; time-resolved photoemission electron microscopy; transition metal dichalcogenides; ultrafast plasmonics}},
  language     = {{eng}},
  number       = {{6}},
  pages        = {{1607--1615}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{ACS Photonics}},
  title        = {{Coherent Excitation and Control of Plasmons on Gold Using Two-Dimensional Transition Metal Dichalcogenides}},
  url          = {{http://dx.doi.org/10.1021/acsphotonics.0c01795}},
  doi          = {{10.1021/acsphotonics.0c01795}},
  volume       = {{8}},
  year         = {{2021}},
}