Plasmon-Mediated Coherent Superposition of Discrete Excitons under Strong Exciton–Plasmon Coupling in Few-Layer MoS2 at Room Temperature
Abstract
In this paper, we demonstrate room temperature coherent hybridization of the A- and B-excitons in few-layer MoS2, mediated by simultaneous strong coupling to surface plasmon polaritons. Few-layer MoS2 was placed on a tunable plasmonic structure and the system’s dispersion was measured by tuning the plasmon energy across the exciton energies. Strong coupling was observed as double Rabi splitting at the A- and B-excitons of 81 and 93 meV, respectively. A coupled harmonic oscillator model sheds light on the nature of the interaction, revealing a quantum superposition of the A- and B-excitons, mediated by the plasmon interaction. This observation suggests the possibility of room temperature intra- or intervalley quantum information transport and/or spin entanglement. The experiment confirms a previous theoretical prediction of room temperature exciton–exciton hybridization in two-dimensional MoS2. Further, through modeling we find that room temperature strong coupling is a general phenomenon among two-dimensional transition metal dichalcogenide exciton–plasmon systems.
- Authors:
-
- National Renewable Energy Lab. (NREL), Golden, CO (United States); Boston College, Chestnut Hill, MA (United States)
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Boston College, Chestnut Hill, MA (United States); Vassar College, Poughkeepsie, NY (United States)
- National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
- Publication Date:
- Research Org.:
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
- OSTI Identifier:
- 1659931
- Report Number(s):
- NREL/JA-5900-74742
Journal ID: ISSN 2330-4022; MainId:6071;UUID:2923dd5c-dfc9-e911-9c26-ac162d87dfe5;MainAdminID:13657
- Grant/Contract Number:
- AC36-08GO28308
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Photonics
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 5; Journal ID: ISSN 2330-4022
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; excitons; MoS2; plasmons; solar fuels; solar-photochemistry; strong coupling; surface plasmon polariton; transition metal dichalcogenide; two-dimensional system
Citation Formats
Rose, Aaron H., Dunklin, Jeremy R., Zhang, Hanyu, Merlo, Juan M., and van de Lagemaat, Jao. Plasmon-Mediated Coherent Superposition of Discrete Excitons under Strong Exciton–Plasmon Coupling in Few-Layer MoS2 at Room Temperature. United States: N. p., 2020.
Web. doi:10.1021/acsphotonics.0c00233.
Rose, Aaron H., Dunklin, Jeremy R., Zhang, Hanyu, Merlo, Juan M., & van de Lagemaat, Jao. Plasmon-Mediated Coherent Superposition of Discrete Excitons under Strong Exciton–Plasmon Coupling in Few-Layer MoS2 at Room Temperature. United States. https://doi.org/10.1021/acsphotonics.0c00233
Rose, Aaron H., Dunklin, Jeremy R., Zhang, Hanyu, Merlo, Juan M., and van de Lagemaat, Jao. Tue .
"Plasmon-Mediated Coherent Superposition of Discrete Excitons under Strong Exciton–Plasmon Coupling in Few-Layer MoS2 at Room Temperature". United States. https://doi.org/10.1021/acsphotonics.0c00233. https://www.osti.gov/servlets/purl/1659931.
@article{osti_1659931,
title = {Plasmon-Mediated Coherent Superposition of Discrete Excitons under Strong Exciton–Plasmon Coupling in Few-Layer MoS2 at Room Temperature},
author = {Rose, Aaron H. and Dunklin, Jeremy R. and Zhang, Hanyu and Merlo, Juan M. and van de Lagemaat, Jao},
abstractNote = {In this paper, we demonstrate room temperature coherent hybridization of the A- and B-excitons in few-layer MoS2, mediated by simultaneous strong coupling to surface plasmon polaritons. Few-layer MoS2 was placed on a tunable plasmonic structure and the system’s dispersion was measured by tuning the plasmon energy across the exciton energies. Strong coupling was observed as double Rabi splitting at the A- and B-excitons of 81 and 93 meV, respectively. A coupled harmonic oscillator model sheds light on the nature of the interaction, revealing a quantum superposition of the A- and B-excitons, mediated by the plasmon interaction. This observation suggests the possibility of room temperature intra- or intervalley quantum information transport and/or spin entanglement. The experiment confirms a previous theoretical prediction of room temperature exciton–exciton hybridization in two-dimensional MoS2. Further, through modeling we find that room temperature strong coupling is a general phenomenon among two-dimensional transition metal dichalcogenide exciton–plasmon systems.},
doi = {10.1021/acsphotonics.0c00233},
journal = {ACS Photonics},
number = 5,
volume = 7,
place = {United States},
year = {Tue Apr 07 00:00:00 EDT 2020},
month = {Tue Apr 07 00:00:00 EDT 2020}
}
Web of Science