Super‐Resolution Lifetime Imaging of Single Molecules Near Gold Bowtie Nanoparticles

Super‐Resolution Lifetime Imaging of Single Molecules Near Gold Bowtie Nanoparticles
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金领结纳米粒子附近单分子的超分辨率寿命成像

DOI:
10.1002/adom.202200480
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发表时间:
2022
影响因子:
9
通讯作者:
Wertz, Esther A.
Wertz, Esther A.
中科院分区:
材料科学2区
文献类型:
--
作者:
Hallenbeck, Zachary;Wertz, Esther A.

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光和物质之间的相互作用是许多技术的基础,但这些设备的质量本质上受到其组成部分的光学特性的限制。等离子体纳米粒子是用于增强此类光学性质的高度通用且可调的平台。然而,这些效应的近场性质使得深入研究和理解这些机制变得困难。在这项工作中,我们介绍了一种完全共聚焦技术结合光开关超分辨率显微镜与荧光寿命成像显微镜研究单分子衰减速率增强。我们证明,该技术结合了优于20 nm的空间分辨率,和16 ps的时间分辨率。同时,还进行了自相关测量,以确认数据确实来源于单分子。这项工作深入了解了等离子体增强发射的各种机制,并允许研究发射强度和寿命增强之间的相关性。这种复杂的关系被证明是依赖于各种辐射和非辐射衰变途径的相对影响。在这里,我们提供了一个平台,用于进一步研究发射错位,不同衰变路径的位置相关的突出,以及局域态密度的直接超分辨测量。
Interactions between light and matter serve as the basis of many technologies, but the quality of these devices is inherently limited by the optical properties of their constituents. Plasmonic nanoparticles are a highly versatile and tunable platform for the enhancement of such optical properties. However, the near‐field nature of these effects has made thorough study and understanding of these mechanisms difficult. In this work, we introduce a fully confocal technique combining photoswitching super‐resolution microscopy with fluorescence lifetime imaging microscopy to study single‐molecule decay rate enhancement. We demonstrate that the technique combines a spatial resolution better than 20 nm, and a 16 ps temporal resolution. Simultaneously, an autocorrelation measurement is also performed to confirm that the data indeed originates from single molecules. This work provides insight into the various mechanisms of plasmon‐enhanced emission, and allows the study of the correlation between emission intensity and lifetime enhancement. This complicated relationship is shown to be dependent upon the relative influence of various radiative and nonradiative decay pathways. Here, we provide a platform for further study of emission mislocalization, the position‐dependent prominence of different decay pathways, and the direct super‐resolved measurement of the local density of states.
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