发射偶极取向揭示溶剂界面处单分子与二维晶体的动态相互作用
Emission dipole orientation reveals dynamic single-molecule interactions with 2D crystals at solvent interfaces
AI总结：
本文提出高通量偏振单分子定位显微镜，同时以纳米精度解析单荧光分子的位置和发射偶极取向，揭示了室温下六方氮化硼与有机溶剂界面处分子相互作用动力学。
摘要：
直接观察单个荧光发射体对于理解和研究量子材料、化学反应和生物系统至关重要。然而，目前的单分子追踪方法仅关注分子的定位，忽略了分子构型和取向。在这项工作中，我们引入了一种高通量偏振单分子定位显微镜，能够同时以纳米精度解析单个荧光发射体的位置和发射偶极取向。利用原始六方氮化硼（h-BN）与有机溶剂之间的界面作为具有挑战性的平台，我们捕获了超过10^5个荧光事件，并揭示了室温下不同的分子相互作用动力学。测得的偶极取向与h-BN晶格的三重旋转对称性一致，液体环境中的分子动力学可以通过电化学调控，这表明了一种按需控制量子发射体的途径。我们还发现，固液界面处的横向扩散比固态发射体更具动态性。这种对分子构型和光物理的同时追踪，增进了对单分子相互作用的理解，并通过二维材料实现了实时传感。
英文摘要：
Direct observation of individual fluorescent emitters is crucial for understanding and studying quantum materials, chemical reactions, and biological systems. However, current single-molecule tracking methods only focuses on the localizations of molecules, overlooking molecular configuration and orientation. In this work, we introduce a high-throughput polarized single-molecule localization microscopy that simultaneously resolves the locations and emission dipole orientations of single fluorescent emitters with nanometer precision. Using the interface between pristine hexagonal boron nitride (h-BN) and an organic solvent as a challenging platform, we capture over 10^5 fluorescent events and reveal distinct molecular interaction dynamics at room temperature. The measured dipole orientations align with the three-fold rotational symmetry of the h-BN lattice, and molecular dynamics in the liquid enivronment can be modulated electrochemically, suggesting a route for on-demand control of quantum emitters. We also find that lateral diffusion at the solid-liquid interface is far more dynamic than that of solid-state emitters. This simultaneous tracking of molecular conformation and photophysics advances the understanding of single-molecule interactions and enables real-time sensing through two-dimensional materials.
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