Chung Kyungwha, Lee Soohyun, Grain Nathan, Moon Kyeongdeuk, Han Seungyeon, Yu Subin, Kang Haeun, Kim Dong Ha, Choi Inhee, Park Sungho, Kim Seokhyoung, Lee Luke P
Institute of Quantum Biophysics, Sungkyunkwan University, Suwon 16419, Republic of Korea.
Department of Medicine, Brigham and Women's Hospital, Harvard Medical School, Harvard University, Boston, Massachusetts 02115, United States.
J Am Chem Soc. 2024 Nov 13;146(45):31150-31158. doi: 10.1021/jacs.4c11083. Epub 2024 Oct 30.
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-. 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.
量子力学被应用于制造众多电子设备,包括激光器、电子显微镜、磁共振成像以及量子信息技术。然而,由于在光学腔与激子物质之间实现强耦合所需的苛刻条件,腔量子电动力学(QED)在各种应用中的实际实现受到限制。在此,我们展示了具有自对准纳米环 doublets 的生物腔 QED:QED-SANDs,它在室温下与生物分子发射体叶绿素 - 表现出稳健的强耦合。我们观察到等离激元 - 激子极化激元的出现,其表现为生物 QED-SANDs 的等离激元散射峰分裂为两个不同的极化激元态,拉比分裂高达约 200 毫电子伏特。我们使用有限元建模阐明了强耦合的机制起源,并通过采用时间耦合模理论量化耦合强度,以获得高达 QED-SANDs 固有衰减率幅度约 3.6 倍的耦合强度。此外,通过室温下的光致发光测量验证了极化激元的稳健存在,从中观察到来自较低极化激元态的强光发射,而来自较高极化激元态的发射被淬灭。QED-SANDs 在深入了解纳米腔中生物分子行为方面具有重大潜力,特别是在量子生物学背景下。