Chemistry Meets Plasmon Polaritons and Cavity Photons

ORAL  · Invited

Abstract

Macroscopic quantum electrodynamics (macroscopic QED) provides a unified framework that integrates the continuum of photonic modes and realistic dielectric environments into molecular systems, offering a comprehensive approach to exploring QED phenomena in chemistry. First, we develop a generalized theory of molecular fluorescence that delivers parameter-free predictions from weak to strong light–matter coupling regimes. Second, we extend resonance energy transfer theory to include both electromagnetic retardation and dielectric responses, yielding improved descriptions of energy transfer mediated by plasmon polaritons and cavity photons. Third, we formulate a unified electron-transfer theory that bridges radiative and non-radiative processes, extend Marcus theory, and demonstrate a wide-dynamic-range control of electron-transfer reactions in the weak-coupling regime. Fourth, we investigate multiple molecules coupled to plasmon polaritons and uncover anomalous giant superradiance that lies beyond the Dicke model. Fifth, we generalize the Born-Huang expansion within the macroscopic QED framework and reveal non-adiabatic QED effects such as non-adiabatic emission, providing insights into QED-driven processes. These advances connect quantum optics, nanophotonics, and chemical physics, offering predictive tools for experimental and theoretical studies on QED chemistry.

*Hsu acknowledges support from Academia Sinica (AS-CDA-111-M02), National Science and Technology Council (111-2113-M-001-027-MY4 and 114-2639-M-002-008-ASP) and Physics Division, and National Center for Theoretical Sciences (112-2124-M-002-003) for the financial support. 

Publication: 1. Hsu, L.-Y.; Chemistry Meets Plasmon Polaritons and Cavity Photons: A Perspective from Macroscopic Quantum Electrodynamics, J. Phys. Chem. Lett., 2025, 16, 1604-1619.
2. Hsu, L.-Y.; Ding, W. D.; Schatz, G. C.; Plasmon-Coupled Resonance Energy Transfer, J. Phys. Chem. Lett., 2017, 8, 2357-2367.
3. Wu, J.-S.; Lin, Y.-C.; Sheu, Y.-L.; Hsu, L.-Y., Characteristic Distance of Resonance Energy Transfer Coupled with Surface Plasmon Polaritons, J. Phys. Chem. Lett., 2018, 9, 7032-7039.
4. Wei, Y.-C.; Lee, M.-W.; Chou, P.-T.; Scholes. G. D.; Schatz, G. C.; Hsu, L.-Y.; Can Nanocavities Significantly Enhance Resonance Energy Transfer in a Single Donor–Acceptor Pair? J. Phys. Chem. C, 2021, 125, 18119-18128.
5. Wang, S; Scholes. G. D.; Hsu, L.-Y.; Quantum Dynamics of a Molecular Emitter Strongly Coupled with Surface Plasmon Polaritons: A Macroscopic Quantum Electrodynamics Approach, J. Chem. Phys., 2019, 151, 014105.
6. Wang, S; Scholes. G. D.; Hsu, L.-Y.; Coherent-to-Incoherent Transition of Molecular Fluorescence Controlled by Surface Plasmon Polaritons, J. Phys. Chem. Lett., 2020, 11, 5948-5955.
7. Wei, Y.-C.; Hsu, L.-Y.; Cavity-Free Quantum-Electrodynamic Electron Transfer Reactions, J. Phys. Chem. Lett., 2022, 13, 9695-9702.
8. Wei, Y.-C.; Hsu, L.-Y.; Wide-Dynamic-Range Control of Quantum-Electrodynamic Electron Transfer Reactions in the Weak Coupling Regime, J. Phys. Chem. Lett., 2024, 15, 7403-7410.
9. Chuang, Y.-T.; Hsu, L.-Y.; Quantum Dynamics of Molecular Ensembles Coupled with Quantum Light: Counter-rotating Interactions as an Essential Component, Phys. Rev. A, 2024, 109, 013717.
10. Chuang, Y.-T.; Hsu, L.-Y.; Anomalous Giant Superradiance in Molecular Aggregates Coupled to Polaritons, Phys. Rev. Lett., 2024, 133, 128001.
11. Tsai, H.-S.; Shen, C.-E.; Hsu, L.-Y.; Generalized Born–Huang Expansion under Macroscopic Quantum Electrodynamics Framework, J. Chem. Phys., 2024, 160, 144112.
12. Shen, C.-E.; Tsai, H.-S.; Hsu, L.-Y.; Non-Adiabatic Quantum Electrodynamic Effects on Electron-Nucleus-Photon Systems: Single Photonic Mode versus Infinite Photonic Modes, J. Chem. Phys., 2025, 162, 034107.
13. Shen, C.-E.; Tsai, H.-S.; Hsu, L.-Y.; Unified Theory of Internal Conversion and Fluorescence under Macroscopic Quantum Electrodynamics Framework, J. Chem. Phys., accepted.








Presenters

  • Liang-Yan Hsu

    • Academia Sinica

Authors

  • Liang-Yan Hsu

    • Academia Sinica