Single-Crystalline Gold Nanodisks on WS2 Mono- and Multilayers for Strong Coupling at Room Temperature

Mathias Geisler, Ximin Cui, Jianfang Wang, Tomas Rindzevicius, Lene Gammelgaard, Bjarke Sørensen Jessen, P. A. D. Gonçalves, Francesco Todisco, Peter Bøggild, Anja Boisen, Martijn Wubs, N. Asger Mortensen, Sanshui Xiao, Nicolas Stenger*

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

Engineering light–matter interactions up to the strong-coupling regime at room temperature is one of the cornerstones of modern nanophotonics. Achieving this goal could enable new platforms for potential applications such as quantum information processing, quantum light sources, and even quantum metrology. Layered materials like transition metal dichalcogenides (TMDCs) and, in particular, tungsten disulfide (WS2), possess strong dipole moments which are comparable to semiconductor-based quantum dots, but the former also exhibit large exciton binding energies, thereby making TMDCs suitable candidates for exploring light–matter interactions at ambient conditions. Furthermore, the combination of TMDCs with plasmonic nanocavities, which tightly confine light down to nanometer scale, has recently emerged as a suitable platform for achieving strong coupling between plasmons and excitons at room temperature. Here, we use ultrathin single-crystalline gold nanodisks featuring large in-plane electric dipole moments aligned with the exciton’s dipole moments in monolayer WS2. By performing both scattering and reflection spectroscopy, we demonstrate strong coupling at room temperature with a Rabi splitting of ∼108 meV. In addition, when the plasmonic resonance of these nanodisks is coupled with few-layer WS2, a Rabi splitting of ∼175 meV is observed, with a major increase of 62% relative to the monolayer configuration. Our results therefore suggest that ultrathin single-crystalline gold nanodisks coupled to WS2 constitute an attractive platform to explore light–matter interactions in the strong-coupling regime.
Original languageEnglish
JournalACS Photonics
Volume6
Pages (from-to)994-1001
ISSN2330-4022
DOIs
Publication statusPublished - 2019

Keywords

  • Plasmonics
  • TMDC
  • WS2
  • Strong coupling
  • Excitons
  • Gold nanodisks

Cite this

@article{1d378b09e4a349ab8439597fb7bf9afd,
title = "Single-Crystalline Gold Nanodisks on WS2 Mono- and Multilayers for Strong Coupling at Room Temperature",
abstract = "Engineering light–matter interactions up to the strong-coupling regime at room temperature is one of the cornerstones of modern nanophotonics. Achieving this goal could enable new platforms for potential applications such as quantum information processing, quantum light sources, and even quantum metrology. Layered materials like transition metal dichalcogenides (TMDCs) and, in particular, tungsten disulfide (WS2), possess strong dipole moments which are comparable to semiconductor-based quantum dots, but the former also exhibit large exciton binding energies, thereby making TMDCs suitable candidates for exploring light–matter interactions at ambient conditions. Furthermore, the combination of TMDCs with plasmonic nanocavities, which tightly confine light down to nanometer scale, has recently emerged as a suitable platform for achieving strong coupling between plasmons and excitons at room temperature. Here, we use ultrathin single-crystalline gold nanodisks featuring large in-plane electric dipole moments aligned with the exciton’s dipole moments in monolayer WS2. By performing both scattering and reflection spectroscopy, we demonstrate strong coupling at room temperature with a Rabi splitting of ∼108 meV. In addition, when the plasmonic resonance of these nanodisks is coupled with few-layer WS2, a Rabi splitting of ∼175 meV is observed, with a major increase of 62{\%} relative to the monolayer configuration. Our results therefore suggest that ultrathin single-crystalline gold nanodisks coupled to WS2 constitute an attractive platform to explore light–matter interactions in the strong-coupling regime.",
keywords = "Plasmonics, TMDC, WS2, Strong coupling, Excitons, Gold nanodisks",
author = "Mathias Geisler and Ximin Cui and Jianfang Wang and Tomas Rindzevicius and Lene Gammelgaard and Jessen, {Bjarke S{\o}rensen} and Gonçalves, {P. A. D.} and Francesco Todisco and Peter B{\o}ggild and Anja Boisen and Martijn Wubs and Mortensen, {N. Asger} and Sanshui Xiao and Nicolas Stenger",
year = "2019",
doi = "10.1021/acsphotonics.8b01766",
language = "English",
volume = "6",
pages = "994--1001",
journal = "A C S Photonics",
issn = "2330-4022",
publisher = "American Chemical Society",

}

Single-Crystalline Gold Nanodisks on WS2 Mono- and Multilayers for Strong Coupling at Room Temperature. / Geisler, Mathias; Cui, Ximin; Wang, Jianfang; Rindzevicius, Tomas; Gammelgaard, Lene; Jessen, Bjarke Sørensen; Gonçalves, P. A. D.; Todisco, Francesco; Bøggild, Peter; Boisen, Anja; Wubs, Martijn; Mortensen, N. Asger; Xiao, Sanshui ; Stenger, Nicolas.

In: ACS Photonics, Vol. 6, 2019, p. 994-1001.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Single-Crystalline Gold Nanodisks on WS2 Mono- and Multilayers for Strong Coupling at Room Temperature

AU - Geisler, Mathias

AU - Cui, Ximin

AU - Wang, Jianfang

AU - Rindzevicius, Tomas

AU - Gammelgaard, Lene

AU - Jessen, Bjarke Sørensen

AU - Gonçalves, P. A. D.

AU - Todisco, Francesco

AU - Bøggild, Peter

AU - Boisen, Anja

AU - Wubs, Martijn

AU - Mortensen, N. Asger

AU - Xiao, Sanshui

AU - Stenger, Nicolas

PY - 2019

Y1 - 2019

N2 - Engineering light–matter interactions up to the strong-coupling regime at room temperature is one of the cornerstones of modern nanophotonics. Achieving this goal could enable new platforms for potential applications such as quantum information processing, quantum light sources, and even quantum metrology. Layered materials like transition metal dichalcogenides (TMDCs) and, in particular, tungsten disulfide (WS2), possess strong dipole moments which are comparable to semiconductor-based quantum dots, but the former also exhibit large exciton binding energies, thereby making TMDCs suitable candidates for exploring light–matter interactions at ambient conditions. Furthermore, the combination of TMDCs with plasmonic nanocavities, which tightly confine light down to nanometer scale, has recently emerged as a suitable platform for achieving strong coupling between plasmons and excitons at room temperature. Here, we use ultrathin single-crystalline gold nanodisks featuring large in-plane electric dipole moments aligned with the exciton’s dipole moments in monolayer WS2. By performing both scattering and reflection spectroscopy, we demonstrate strong coupling at room temperature with a Rabi splitting of ∼108 meV. In addition, when the plasmonic resonance of these nanodisks is coupled with few-layer WS2, a Rabi splitting of ∼175 meV is observed, with a major increase of 62% relative to the monolayer configuration. Our results therefore suggest that ultrathin single-crystalline gold nanodisks coupled to WS2 constitute an attractive platform to explore light–matter interactions in the strong-coupling regime.

AB - Engineering light–matter interactions up to the strong-coupling regime at room temperature is one of the cornerstones of modern nanophotonics. Achieving this goal could enable new platforms for potential applications such as quantum information processing, quantum light sources, and even quantum metrology. Layered materials like transition metal dichalcogenides (TMDCs) and, in particular, tungsten disulfide (WS2), possess strong dipole moments which are comparable to semiconductor-based quantum dots, but the former also exhibit large exciton binding energies, thereby making TMDCs suitable candidates for exploring light–matter interactions at ambient conditions. Furthermore, the combination of TMDCs with plasmonic nanocavities, which tightly confine light down to nanometer scale, has recently emerged as a suitable platform for achieving strong coupling between plasmons and excitons at room temperature. Here, we use ultrathin single-crystalline gold nanodisks featuring large in-plane electric dipole moments aligned with the exciton’s dipole moments in monolayer WS2. By performing both scattering and reflection spectroscopy, we demonstrate strong coupling at room temperature with a Rabi splitting of ∼108 meV. In addition, when the plasmonic resonance of these nanodisks is coupled with few-layer WS2, a Rabi splitting of ∼175 meV is observed, with a major increase of 62% relative to the monolayer configuration. Our results therefore suggest that ultrathin single-crystalline gold nanodisks coupled to WS2 constitute an attractive platform to explore light–matter interactions in the strong-coupling regime.

KW - Plasmonics

KW - TMDC

KW - WS2

KW - Strong coupling

KW - Excitons

KW - Gold nanodisks

U2 - 10.1021/acsphotonics.8b01766

DO - 10.1021/acsphotonics.8b01766

M3 - Journal article

VL - 6

SP - 994

EP - 1001

JO - A C S Photonics

JF - A C S Photonics

SN - 2330-4022

ER -