Plasmon-Mediated Coherent Superposition of Discrete Excitons under Strong Exciton–Plasmon Coupling in Few-Layer MoS2 at Room Temperature

Rose, Aaron H.; Dunklin, Jeremy R.; Zhang, Hanyu; Merlo, Juan M.; van de Lagemaat, Jao

doi:10.1021/acsphotonics.0c00233

Title: Plasmon-Mediated Coherent Superposition of Discrete Excitons under Strong Exciton–Plasmon Coupling in Few-Layer MoS₂ at Room Temperature

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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:

^[1];

^[2];

^[2]; Merlo, Juan M. ^[3];

^[4]

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:: Tue Apr 07 00:00:00 EDT 2020

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.

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                    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

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                    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.

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@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}

}

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Title: Plasmon-Mediated Coherent Superposition of Discrete Excitons under Strong Exciton–Plasmon Coupling in Few-Layer MoS2 at Room Temperature

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Title: Plasmon-Mediated Coherent Superposition of Discrete Excitons under Strong Exciton–Plasmon Coupling in Few-Layer MoS₂ at Room Temperature