Electrochemical Control of Strong Coupling of CdSe Exciton-Polaritons in Plasmonic Cavities

Nathan G. Sinai; Christian Y. Dones Lassalle; Jennica E. Kelm; Shreya K. Patel; Sang Min Park; Max J.H. Tan; Teri W. Odom; Jillian L. Dempsey

doi:10.1021/acs.nanolett.4c01790

Electrochemical Control of Strong Coupling of CdSe Exciton-Polaritons in Plasmonic Cavities

Nathan G. Sinai, Christian Y. Dones Lassalle, Jennica E. Kelm, Shreya K. Patel, Sang Min Park, Max J.H. Tan, Teri W. Odom^*, Jillian L. Dempsey^*

^*Corresponding author for this work

Chemistry

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

3 Scopus citations

Abstract

This work reports in situ (active) electrochemical control over the coupling strength between semiconducting nanoplatelets and a plasmonic cavity. We found that by applying a reductive bias to an Al nanoparticle lattice working electrode the number of CdSe nanoplatelet emitters that can couple to the cavity is decreased. Strong coupling can be reversibly recovered by discharging the lattice at oxidative potentials relative to the conduction band edge reduction potential of the emitters. By correlating the number of electrons added or removed with the measured coupling strength, we identified that loss and recovery of strong coupling are likely hindered by side processes that trap and/or inhibit electrons from populating the nanoplatelet conduction band. These findings demonstrate tunable, external control of strong coupling and offer prospects to tune selectivity in chemical reactions.

Original language	English (US)
Pages (from-to)	7491-7498
Number of pages	8
Journal	Nano letters
Volume	24
Issue number	24
DOIs	https://doi.org/10.1021/acs.nanolett.4c01790
State	Published - Jun 19 2024

Funding

The research was supported by the National Science Foundation (NSF) Center for Quantum Electrodynamics for Selective Transformations (QuEST) (CHE-2124398). T.W.O. acknowledges support from the Vannevar Bush Faculty Fellowship from the U.S. Department of Defense (DOD N00014-17-1-3023). This work made use of the NUFAB, EPIC, and SPID facilities of Northwestern University\u2019s NUANCE Center that has received support from the SHyNE Resource (NSF ECCS-2025633), the International Institute for Nanotechnology at Northwestern University (IIN), Northwestern\u2019s MRSEC Program (NSF DMR-1720139), and MRI (NSF DMR-1828676). S.K.P. acknowledges support from the NSF MPS-Ascend Postdoctoral Research Fellowship (CHE-2316063). S.-M.P. and M.J.H.T. gratefully acknowledge support from the Ryan Fellowship and the International Institute for Nanotechnology at Northwestern University. This research was supported in part by the Quest high performance computing facility at Northwestern University, which is jointly supported by the Office of the Provost, the Office for Research, and Northwestern University Information Technology. We thank Francisco Freire Fernandez and Alex Sample at Northwestern University, Todd Krauss at University of Rochester, Neil Spinner and Alex Peroff from Pine Research, and Alexandria Bredar from the University of North Carolina at Chapel Hill for their assistance with this project and insightful discussions.

Keywords

CdSe nanoplatelets
electrochemical control
exciton-polariton
nanoparticle lattice cavity

ASJC Scopus subject areas

Bioengineering
General Chemistry
General Materials Science
Condensed Matter Physics
Mechanical Engineering

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10.1021/acs.nanolett.4c01790

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title = "Electrochemical Control of Strong Coupling of CdSe Exciton-Polaritons in Plasmonic Cavities",

abstract = "This work reports in situ (active) electrochemical control over the coupling strength between semiconducting nanoplatelets and a plasmonic cavity. We found that by applying a reductive bias to an Al nanoparticle lattice working electrode the number of CdSe nanoplatelet emitters that can couple to the cavity is decreased. Strong coupling can be reversibly recovered by discharging the lattice at oxidative potentials relative to the conduction band edge reduction potential of the emitters. By correlating the number of electrons added or removed with the measured coupling strength, we identified that loss and recovery of strong coupling are likely hindered by side processes that trap and/or inhibit electrons from populating the nanoplatelet conduction band. These findings demonstrate tunable, external control of strong coupling and offer prospects to tune selectivity in chemical reactions.",

keywords = "CdSe nanoplatelets, electrochemical control, exciton-polariton, nanoparticle lattice cavity",

author = "Sinai, {Nathan G.} and {Dones Lassalle}, {Christian Y.} and Kelm, {Jennica E.} and Patel, {Shreya K.} and Park, {Sang Min} and Tan, {Max J.H.} and Odom, {Teri W.} and Dempsey, {Jillian L.}",

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AU - Sinai, Nathan G.

AU - Dones Lassalle, Christian Y.

AU - Kelm, Jennica E.

AU - Patel, Shreya K.

AU - Park, Sang Min

AU - Tan, Max J.H.

AU - Odom, Teri W.

AU - Dempsey, Jillian L.

PY - 2024/6/19

Y1 - 2024/6/19

N2 - This work reports in situ (active) electrochemical control over the coupling strength between semiconducting nanoplatelets and a plasmonic cavity. We found that by applying a reductive bias to an Al nanoparticle lattice working electrode the number of CdSe nanoplatelet emitters that can couple to the cavity is decreased. Strong coupling can be reversibly recovered by discharging the lattice at oxidative potentials relative to the conduction band edge reduction potential of the emitters. By correlating the number of electrons added or removed with the measured coupling strength, we identified that loss and recovery of strong coupling are likely hindered by side processes that trap and/or inhibit electrons from populating the nanoplatelet conduction band. These findings demonstrate tunable, external control of strong coupling and offer prospects to tune selectivity in chemical reactions.

AB - This work reports in situ (active) electrochemical control over the coupling strength between semiconducting nanoplatelets and a plasmonic cavity. We found that by applying a reductive bias to an Al nanoparticle lattice working electrode the number of CdSe nanoplatelet emitters that can couple to the cavity is decreased. Strong coupling can be reversibly recovered by discharging the lattice at oxidative potentials relative to the conduction band edge reduction potential of the emitters. By correlating the number of electrons added or removed with the measured coupling strength, we identified that loss and recovery of strong coupling are likely hindered by side processes that trap and/or inhibit electrons from populating the nanoplatelet conduction band. These findings demonstrate tunable, external control of strong coupling and offer prospects to tune selectivity in chemical reactions.

KW - CdSe nanoplatelets

KW - electrochemical control

KW - exciton-polariton

KW - nanoparticle lattice cavity

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Electrochemical Control of Strong Coupling of CdSe Exciton-Polaritons in Plasmonic Cavities

Abstract

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Keywords

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