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PreprintCC BYChemRxiv

There is Room in the Middle: Unidirectional Energy Transfer in Plasmonic Nanohybrids through Intermediate Coherence

  • Hyuncheol Oh1,2
  • Md Ashiqur Rahman3,4
  • Jaekak Yoo1,2
  • Emily A. Cook1,2
  • Diana Soto3,4
  • Zhenyang Jia3,4
  • Tinglian Yuan1,2
  • Jae-Myoung Kim1,2
  • Katsuya Shiratori5,2
  • Catherine J. Murphy1,2
  • Stephan Link1,2,6
  • Christy F. Landes1,2,3,4,6
6 affiliations
  1. 1Department of Chemistry
  2. 2University of Illinois Urbana-Champaign
  3. 3Department of Chemical and Biomolecular Engineering
  4. 4University of Illinois Urbana-
  5. 5Department of Physics
  6. 6Department of Electrical and Computer Engineering
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Abstract

Plasmon-induced resonance energy transfer (PIRET) is less well-known than hot carrier and polaritonic photocatalysis. The small dipole moment of individual excitons means donors and acceptors are weakly coupled in molecular energy transfer, so it is considered not efficient as hot carrier photocatalysis. And unlike the detailed quantum descriptions for polaritons in vibrational and electronic strong coupling, there is not a clear mechanistic model for PIRET. Here, we establish the underlying mechanism of PIRET and show energy transfer efficiencies of up to 75%. Gold nanorod (AuNR)-methylene blue polymer nanohybrids with identical plasmon resonance energies but with systematically varied core sizes enable direct comparison of the competing roles of oscillator strength and dephasing. Operando single-particle spectroelectrochemistry is used to quantify PIRET efficiencies. Open-quantum and classical electrodynamics simulations reveal that smaller AuNRs have an advantage because they combine stronger eigenmode-normalized local coupling with slower plasmon dephasing. PIRET efficiency increases from 30% to 75% with optimized AuNR sizes. The unique oscillator properties of AuNRs establish intermediate coherence, between more familiar weakly and strongly coupled regimes, as an effective route to unidirectional plasmon-to-exciton transfer. Intermediate coherence is a kinetic gate for PIRET, creating an efficient way to transform light into chemical degrees of freedom through which further photocatalysis is possible.

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Cite

BibTeXRIS
BibTeX
@misc{oh2026there,
  title = {{There is Room in the Middle: Unidirectional Energy Transfer in Plasmonic Nanohybrids through Intermediate Coherence}},
  author = {Hyuncheol Oh and Md Ashiqur Rahman and Jaekak Yoo and Emily A. Cook and Diana Soto and Zhenyang Jia and Tinglian Yuan and Jae-Myoung Kim and Katsuya Shiratori and Catherine J. Murphy and Stephan Link and Christy F. Landes},
  howpublished = {ChemRxiv},
  year = {2026},
  month = sep,
  doi = {10.26434/chemrxiv.15009067/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009067/v1},
  note = {CC BY},
}
RIS
TY  - UNPB
TI  - There is Room in the Middle: Unidirectional Energy Transfer in Plasmonic Nanohybrids through Intermediate Coherence
AU  - Hyuncheol Oh
AU  - Md Ashiqur Rahman
AU  - Jaekak Yoo
AU  - Emily A. Cook
AU  - Diana Soto
AU  - Zhenyang Jia
AU  - Tinglian Yuan
AU  - Jae-Myoung Kim
AU  - Katsuya Shiratori
AU  - Catherine J. Murphy
AU  - Stephan Link
AU  - Christy F. Landes
PY  - 2026
DA  - 2026/09/18
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15009067/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009067/v1
AB  - Plasmon-induced resonance energy transfer (PIRET) is less well-known than hot carrier and polaritonic photocatalysis. The small dipole moment of individual excitons means donors and acceptors are weakly coupled in molecular energy transfer, so it is considered not efficient as hot carrier photocatalysis. And unlike the detailed quantum descriptions for polaritons in vibrational and electronic strong coupling, there is not a clear mechanistic model for PIRET. Here, we establish the underlying mechanism of PIRET and show energy transfer efficiencies of up to 75%. Gold nanorod (AuNR)-methylene blue polymer nanohybrids with identical plasmon resonance energies but with systematically varied core sizes enable direct comparison of the competing roles of oscillator strength and dephasing. Operando single-particle spectroelectrochemistry is used to quantify PIRET efficiencies. Open-quantum and classical electrodynamics simulations reveal that smaller AuNRs have an advantage because they combine stronger eigenmode-normalized local coupling with slower plasmon dephasing. PIRET efficiency increases from 30% to 75% with optimized AuNR sizes. The unique oscillator properties of AuNRs establish intermediate coherence, between more familiar weakly and strongly coupled regimes, as an effective route to unidirectional plasmon-to-exciton transfer. Intermediate coherence is a kinetic gate for PIRET, creating an efficient way to transform light into chemical degrees of freedom through which further photocatalysis is possible.
ER  -