二维过渡金属二硫属化合物中反应性硫空位的超分辨光学映射
Super-resolved optical mapping of reactive sulfur-vacancy in 2D transition metal dichalcogenides
摘要：
过渡金属二硫属化物（TMD）代表了一类全新的半导体二维材料，具有令人兴奋的性能。2D TMD中的缺陷会严重影响其物理和化学性能。然而，缺陷的存在和空间分布的表征在吞吐量或分辨率方面受到限制。在这里，我们展示了大面积映射的反应性硫缺乏缺陷的二维TMDs耦合单分子定位显微镜与荧光标记，使用硫醇化学。我们的方法，让人想起PAINT策略，依赖于通过可逆的物理吸附的荧光探针的硫空位通过硫醇基团和它们的间歇性发射的特异性结合，以应用本地化的标记的缺陷的精度下降到15 nm。调节荧光团和对接巯基位点之间的距离使我们能够控制Föster共振能量转移（FRET）过程，并揭示由于局部不规则晶格结构而导致的大的结构缺陷，如晶界和线缺陷。我们的方法提供了一个简单而快速的替代大规模映射的非辐射缺陷的二维材料，并铺平了道路，原位和空间分辨监测化学试剂和二维材料中的缺陷之间的相互作用，具有一般意义的缺陷工程在水的条件。
英文摘要：
Transition metal dichalcogenides (TMDs) represent an entire new class of semiconducting 2D materials with exciting properties. Defects in 2D TMDs can crucially affect their physical and chemical properties. However, characterization of the presence and spatial distribution of defects is limited either in throughput or in resolution. Here, we demonstrate large area mapping of reactive sulfur-deficient defects in 2D-TMDs coupling single-molecule localization microscopy with fluorescence labeling using thiol chemistry. Our method, reminiscent of PAINT strategies, relies on the specific binding by reversible physisorption of fluorescent probes to sulfur-vacancies via a thiol group and their intermittent emission to apply localization of the labeled defects with a precision down to 15 nm. Tuning the distance between the fluorophore and the docking thiol site allows us to control Föster Resonance Energy Transfer (FRET) process and reveal large structural defects such as grain boundaries and line defects, due to the local irregular lattice structure. Our methodology provides a simple and fast alternative for large-scale mapping of non-radiative defects in 2D materials and paves the way for in-situ and spatially resolved monitoring of the interaction between chemical agent and the defects in 2D materials that has general implications for defect engineering in aqueous condition.
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