TY - JOUR
T1 - Biological Cavity Quantum Electrodynamics via Self-Aligned Nanoring Doublets
T2 - QED-SANDs
AU - Chung, Kyungwha
AU - Lee, Soohyun
AU - Grain, Nathan
AU - Moon, Kyeongdeuk
AU - Han, Seungyeon
AU - Yu, Subin
AU - Kang, Haeun
AU - Kim, Dong Ha
AU - Choi, Inhee
AU - Park, Sungho
AU - Kim, Seokhyoung
AU - Lee, Luke P.
N1 - Publisher Copyright:
© 2024 American Chemical Society.
PY - 2024/11/13
Y1 - 2024/11/13
N2 - Quantum mechanics is applied to create numerous electronic devices, including lasers, electron microscopes, magnetic resonance imaging, and quantum information technology. However, the practical realization of cavity quantum electrodynamics (QED) in various applications is limited due to the demanding conditions required for achieving strong coupling between an optical cavity and excitonic matter. Here, we present biological cavity QED with self-aligned nanoring doublets: QED-SANDs, which exhibit robust room-temperature strong coupling with a biomolecular emitter, chlorophyll-a. We observe the emergence of plasmon-exciton polaritons, which manifest as a bifurcation of the plasmonic scattering peak of biological QED-SANDs into two distinct polariton states with Rabi splitting up to ∼200 meV. We elucidate the mechanistic origin of strong coupling using finite-element modeling and quantify the coupling strength by employing temporal coupled-mode theory to obtain the coupling strength up to approximately 3.6 times the magnitude of the intrinsic decay rate of QED-SANDs. Furthermore, the robust presence of the polaritons is verified through photoluminescence measurements at room temperature, from which strong light emission from the lower polariton state is observed, while emission from the upper polariton state is quenched. QED-SANDs present significant potential for groundbreaking insights into biomolecular behavior in nanocavities, especially in the context of quantum biology.
AB - Quantum mechanics is applied to create numerous electronic devices, including lasers, electron microscopes, magnetic resonance imaging, and quantum information technology. However, the practical realization of cavity quantum electrodynamics (QED) in various applications is limited due to the demanding conditions required for achieving strong coupling between an optical cavity and excitonic matter. Here, we present biological cavity QED with self-aligned nanoring doublets: QED-SANDs, which exhibit robust room-temperature strong coupling with a biomolecular emitter, chlorophyll-a. We observe the emergence of plasmon-exciton polaritons, which manifest as a bifurcation of the plasmonic scattering peak of biological QED-SANDs into two distinct polariton states with Rabi splitting up to ∼200 meV. We elucidate the mechanistic origin of strong coupling using finite-element modeling and quantify the coupling strength by employing temporal coupled-mode theory to obtain the coupling strength up to approximately 3.6 times the magnitude of the intrinsic decay rate of QED-SANDs. Furthermore, the robust presence of the polaritons is verified through photoluminescence measurements at room temperature, from which strong light emission from the lower polariton state is observed, while emission from the upper polariton state is quenched. QED-SANDs present significant potential for groundbreaking insights into biomolecular behavior in nanocavities, especially in the context of quantum biology.
UR - http://www.scopus.com/inward/record.url?scp=85208409532&partnerID=8YFLogxK
U2 - 10.1021/jacs.4c11083
DO - 10.1021/jacs.4c11083
M3 - Article
C2 - 39475264
AN - SCOPUS:85208409532
SN - 0002-7863
VL - 146
SP - 31150
EP - 31158
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 45
ER -