Zhang Yao, Yang Ben, Ghafoor Atif, Zhang Yang, Zhang Yu-Fan, Wang Rui-Pu, Yang Jin-Long, Luo Yi, Dong Zhen-Chao, Hou J G
Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei 230026, China.
Natl Sci Rev. 2019 Nov;6(6):1169-1175. doi: 10.1093/nsr/nwz180. Epub 2019 Nov 8.
The strong spatial confinement of a nanocavity plasmonic field has made it possible to visualize the inner structure of a single molecule and even to distinguish its vibrational modes in real space. With such ever-improved spatial resolution, it is anticipated that full vibrational imaging of a molecule could be achieved to reveal molecular structural details. Here we demonstrate full Raman images of individual vibrational modes at the ångström level for a single Mg-porphine molecule, revealing distinct characteristics of each vibrational mode in real space. Furthermore, by exploiting the underlying interference effect and Raman fingerprint database, we propose a new methodology for structural determination, which we have called 'scanning Raman picoscopy', to show how such ultrahigh-resolution spectromicroscopic vibrational images can be used to visually assemble the chemical structure of a single molecule through a simple Lego-like building process.
纳米腔等离子体激元场的强空间限制使得可视化单个分子的内部结构甚至在实空间中区分其振动模式成为可能。随着空间分辨率的不断提高，预计可以实现分子的全振动成像以揭示分子结构细节。在这里，我们展示了单个镁卟啉分子在埃级别的各个振动模式的全拉曼图像，揭示了每个振动模式在实空间中的独特特征。此外，通过利用潜在的干涉效应和拉曼指纹数据库，我们提出了一种新的结构确定方法，我们称之为“扫描拉曼皮秒显微镜术”，以展示如何通过一个简单的类似乐高积木的构建过程，利用这种超高分辨率光谱显微镜振动图像直观地组装单个分子的化学结构。
