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Locating Single-Atom Optical Picocavities Using Wavelength-Multiplexed Raman Scattering
ACS Photonics ( IF 6.5 ) Pub Date : 2021-10-04 , DOI: 10.1021/acsphotonics.1c01100 Jack Griffiths 1 , Bart de Nijs 1 , Rohit Chikkaraddy 1 , Jeremy J Baumberg 1
ACS Photonics ( IF 6.5 ) Pub Date : 2021-10-04 , DOI: 10.1021/acsphotonics.1c01100 Jack Griffiths 1 , Bart de Nijs 1 , Rohit Chikkaraddy 1 , Jeremy J Baumberg 1
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Transient atomic protrusions in plasmonic nanocavities confine optical fields to sub-1-nm3 picocavities, allowing the optical interrogation of single molecules at room temperature. While picocavity formation is linked to both the local chemical environment and optical irradiation, the role of light in localizing the picocavity formation is unclear. Here, we combine information from thousands of picocavity events and simultaneously compare the transient Raman scattering arising from two incident pump wavelengths. Full analysis of the data set suggests that light suppresses the local effective barrier height for adatom formation and that the initial barrier height is decreased by reduced atomic coordination numbers near facet edges. Modeling the system also resolves the frequency-dependent picocavity field enhancements supported by these atomic scale features.
中文翻译：
使用波长复用拉曼散射定位单原子光学皮腔
等离子体纳米腔中的瞬态原子突起将光场限制在亚 1 纳米3皮腔，允许在室温下对单个分子进行光学询问。虽然皮腔形成与局部化学环境和光辐射有关，但光在局部化皮腔形成中的作用尚不清楚。在这里，我们结合了来自数千个皮腔事件的信息，并同时比较了由两个入射泵浦波长引起的瞬态拉曼散射。对数据集的全面分析表明，光抑制了吸附原子形成的局部有效势垒高度，并且初始势垒高度因小平面边缘附近原子配位数的减少而降低。系统建模还解决了这些原子尺度特征支持的频率相关皮腔场增强问题。
更新日期：2021-10-20
中文翻译：
使用波长复用拉曼散射定位单原子光学皮腔
等离子体纳米腔中的瞬态原子突起将光场限制在亚 1 纳米3皮腔，允许在室温下对单个分子进行光学询问。虽然皮腔形成与局部化学环境和光辐射有关，但光在局部化皮腔形成中的作用尚不清楚。在这里，我们结合了来自数千个皮腔事件的信息，并同时比较了由两个入射泵浦波长引起的瞬态拉曼散射。对数据集的全面分析表明，光抑制了吸附原子形成的局部有效势垒高度，并且初始势垒高度因小平面边缘附近原子配位数的减少而降低。系统建模还解决了这些原子尺度特征支持的频率相关皮腔场增强问题。
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