通过自对准纳米双星实现生物腔量子电动力学:QED-SANDs

IF 14.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Journal of the American Chemical Society Pub Date : 2024-10-30 DOI:10.1021/jacs.4c11083
Kyungwha Chung, Soohyun Lee, Nathan Grain, Kyeongdeuk Moon, Seungyeon Han, Subin Yu, Haeun Kang, Dong Ha Kim, Inhee Choi, Sungho Park, Seokhyoung Kim, Luke P. Lee
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引用次数: 0

摘要

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、磁共振成像和量子信息技术。然而,由于实现光腔与激子物质之间的强耦合需要苛刻的条件,腔量子电动力学(QED)在各种应用中的实际实现受到了限制。在此,我们提出了具有自对准纳米双核的生物空腔量子电动力学:QED-SANDs,它与生物分子发射体叶绿素-a 之间表现出了强大的室温强耦合。我们观察到质子-激子极化子的出现,它表现为生物 QED-SAND 的质子散射峰分叉为两个不同的极化子态,拉比分裂高达 ∼200 meV。我们利用有限元建模阐明了强耦合的机理起源,并利用时态耦合模式理论量化了耦合强度,得到的耦合强度约为 QED-SAND 固有衰减率的 3.6 倍。此外,通过室温下的光致发光测量验证了极化子的稳健存在,从中观察到下极化子态的强光发射,而上极化子态的发射被淬灭。QED-SANDs 具有巨大的潜力,可以让人们对纳米腔中的生物分子行为,尤其是量子生物学方面的生物分子行为有突破性的了解。
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Biological Cavity Quantum Electrodynamics via Self-Aligned Nanoring Doublets: QED-SANDs
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.
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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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