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Subgroup 3 On-Surface Synthesis and Single-Molecule Characterization

2025-04-23

借助扫描隧道显微镜STM等表面科学技术,表面合成化学近年来迅猛发展,一些利用传统方法无法获得的低维碳基纳米结构得到了精确制备。通过对前驱体分子的合理设计、热力学动力学调控、自旋态保护、针尖操纵等方法,一些具有奇异自旋和拓扑性质的碳结构也有望通过表面合成的方法得到原子级精准制备和表征。此外,将STM与制备级质谱、同步辐射技术等多种手段联用,也有望实现溶液反应机理研究的突破,在单原子尺度实现反应中间体精确解构,从而明晰反应机理。围绕上述设想,基于表面化学和溶液化学的深度融合,团队研究主要围绕以下两个方面展开:

(1)自旋拓扑碳结构的合成与表征。利用表面合成化学的手段,借助扫描隧道显微镜/显微谱、非接触式原子力显微镜和高分辨同步辐射谱学技术,进行低维自旋碳结构的原子级精准构筑和相应自旋态、拓扑态的单分子尺度表征和解析,并探索其在电子器件中的应用。

(2)有机反应中间体表征。发展质谱分离-STM-同步辐射谱学-针尖增强拉曼多维度表征系统,将溶液反应中复杂中间体利用软着陆的方法沉积到样品靶面上,通过STM对其结构进行亚原子尺度成像,通过STM针尖与同步辐射耦合对其元素和价态进行单原子尺度辨认,通过针尖增强拉曼对其官能团进行埃级分辨识别,从而明确中间体结构,明晰有机反应机理。


Recent advancements in surface science technologies, such as scanning tunneling microscopy (STM), have significantly accelerated the development of surface synthetic chemistry. This progress has enabled the precise fabrication of low-dimensional carbon-based nanostructures that are unattainable through traditional methodologies. By employing rational design of precursor molecules, thermodynamic and kinetic regulation, spin state protection, and tip manipulation, researchers can anticipate the precise preparation and characterization of carbon nanostructures exhibiting unique spin and topological properties at the atomic level via on-surface synthesis.

Moreover, integrating STM with preparative mass spectrometry and synchrotron radiation technology is expected to enhance the investigation of solution reaction mechanisms, facilitating the accurate dissection of reaction intermediates at the single-atom scale and thereby elucidating the underlying reaction mechanisms.

In light of these concepts and the synergistic integration of surface and solution chemistry, the research team is concentrating on the following two primary avenues:

1. **Synthesis and Characterization of Spin Topological Carbon Structures**: Utilizing surface synthetic chemistry, scanning tunneling microscopy/spectroscopy, non-contact atomic force microscopy, and high-resolution synchrotron radiation spectroscopy, our study aims to achieve atomic-level precision in the construction of low-dimensional spin carbon structures and to characterize the corresponding spin states and topological states at the single-molecule scale.

2. **Characterization of Organic Reaction Intermediates**: We will develop a mass spectrometry separation-STM-synchrotron radiation spectroscopy-tip enhanced Raman multi-dimensional characterization system for the characterization of organic reaction intermediates at single-molecule level.  The complex reaction intermediates are deposited from solution reactions onto surfaces via soft landing. Their structures will be imaged at the subatomic scale using STM, while element identification and valence state assessment will be conducted at the single-atom level through the coupling of the STM tip with synchrotron radiation. Functional group identification at the angstrom level will be achieved through tip enhanced Raman spectroscopy. This system allows for the clarification of structures of intermediates thereby elucidating the mechanisms of organic reactions.



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