4.8 Article

Quantum Electrodynamic Behavior of Chlorophyll in a Plasmonic Nanocavity

Journal

NANO LETTERS
Volume 22, Issue 24, Pages 9861-9868

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.2c02917

Keywords

quantum electrodynamics; chlorophyll; plasmonics; nanocavity; strong coupling; energy splitting

Funding

  1. Air Force Office of Scientific Research Grant [AFOSR FA2386-20-1-4060]
  2. HK Lee Foundation for the Institute of Quantum Biophysics
  3. Department of Biophysics at Sungkyunkwan University
  4. National Research Foundation of Korea - Ministry of Science, ICT, and Future Planning [NRF-2020R1A2C2005760, NRF-2020R1A2C3012167]

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This study reports the quantum electrodynamic behavior of chlorophyll-a in a plasmonic nanocavity. By constructing an extreme plasmonic nanocavity and using hyperspectral imaging technology, the energy level splitting of chlorophyll-a was observed. This study provides important insights for further exploration in quantum biological electron or energy transfer, electrodynamics, and other fields.
Plasmonic nanocavities have been used as a novel platform for studying strong light-matter coupling, opening access to quantum chemistry, material science, and enhanced sensing. However, the biomolecular study of cavity quantum electrodynamics (QED) is lacking. Here, we report the quantum electrodynamic behavior of chlorophyll-a in a plasmonic nanocavity. We construct an extreme plasmonic nanocavity using Au nanocages with various linker molecules and Au mirrors to obtain a strong coupling regime. Plasmon resonance energy transfer (PRET)-based hyperspectral imaging is applied to study the electrodynamic behaviors of chlorophyll-a in the nanocavity. Furthermore, we observe the energy level splitting of chlorophyll-a, similar to the cavity QED effects due to the light- matter interactions in the cavity. Our study will provide insight for further studies in quantum biological electron or energy transfer, electrodynamics, the electron transport chain of mitochondria, and energy harvesting, sensing, and conversion in both biological and biophysical systems.

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