Decoherence Tuning in Voltage-Driven Plasmonic Cavities
Abstract
Strong light-matter coupling offers a powerful framework for modifying molecular structure, dynamics, and optical response, yet achieving this regime at the single-molecule level remains a central challenge. Scanning Tunneling Microscope Break Junctions (STM-BJ) provide a promising route by combining single-molecule addressability with extreme nanoscale field confinement. However, the metallic environment that enables such confinement also introduces substantial plasmonic and excitonic losses, raising the question of how strong coupling can be realized in a metal-molecule-metal junction. Here, we identify the voltage as the key control parameter. We show that the applied bias not only drives the formation of an interfacial exciton through resonant charge transport but also suppresses its coupling to metallic loss channels. Simultaneously, the plasmonic cavity retains extreme mode confinement while the availability of modes is moderately tuned by voltage. Together, these results establish voltage-driven STM-BJs as electrically tunable single-molecule plasmonic cavities and open new routes for using the powerful STM-BJ toolbox, including quantum transport, tracking chemical dynamics, optoelectronics, and molecular-scale quantum control under strong light-matter coupling.
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BibTeX
@misc{wang2026decoherence,
title = {{Decoherence Tuning in Voltage-Driven Plasmonic Cavities}},
author = {Yuchen Wang and Oliver Tan and Norah M. Hoffmann},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.28287},
eprint = {2609.28287},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.28287},
}
RIS
TY - UNPB
TI - Decoherence Tuning in Voltage-Driven Plasmonic Cavities
AU - Yuchen Wang
AU - Oliver Tan
AU - Norah M. Hoffmann
PY - 2026
DA - 2026/09/23
PB - arXiv
DO - 10.48550/arxiv.2609.28287
UR - https://arxiv.org/abs/2609.28287
AB - Strong light-matter coupling offers a powerful framework for modifying molecular structure, dynamics, and optical response, yet achieving this regime at the single-molecule level remains a central challenge. Scanning Tunneling Microscope Break Junctions (STM-BJ) provide a promising route by combining single-molecule addressability with extreme nanoscale field confinement. However, the metallic environment that enables such confinement also introduces substantial plasmonic and excitonic losses, raising the question of how strong coupling can be realized in a metal-molecule-metal junction. Here, we identify the voltage as the key control parameter. We show that the applied bias not only drives the formation of an interfacial exciton through resonant charge transport but also suppresses its coupling to metallic loss channels. Simultaneously, the plasmonic cavity retains extreme mode confinement while the availability of modes is moderately tuned by voltage. Together, these results establish voltage-driven STM-BJs as electrically tunable single-molecule plasmonic cavities and open new routes for using the powerful STM-BJ toolbox, including quantum transport, tracking chemical dynamics, optoelectronics, and molecular-scale quantum control under strong light-matter coupling.
ER -