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arXiv · 2408.01207

Emission dipole orientation reveals dynamic single-molecule interactions with 2D crystals at solvent interfaces

Wei Guo·Tzu-Heng Chen·Nathan Ronceray·Eveline Mayner·Kenji Watanabe·Takashi Taniguchi·Aleksandra Radenovic
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Abstract

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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Wei Guo, Tzu-Heng Chen, Nathan Ronceray, Eveline Mayner, Kenji Watanabe, Takashi Taniguchi, Aleksandra Radenovic. 2024-08-02. Emission dipole orientation reveals dynamic single-molecule interactions with 2D crystals at solvent interfaces. https://doi.org/10.1038/s41467-026-74191-w

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