期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 12, 期 7, 页码 1961-1968出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.1c00074
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资金
- National Key R&D Program of China [2016YFA0200600, 2017YFA0303500]
- National Natural Science Foundation of China
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB36000000]
- Anhui Initiative in Quantum Information Technologies
- Young Scholars Program of Shandong University [2018WLJH49]
In this work, we demonstrated real-time tracking of bond breaking and making processes of an up-standing melamine molecule chemisorbed on Cu(100) using subnanometer resolved tip-enhanced Raman spectroscopy (TERS). The results indicate the chemical and structural sensitivity of TERS for single-molecule recognition beyond flat-lying planar molecules.
Probing bond breaking and making as well as related structural changes at the single-molecule level is of paramount importance for understanding the mechanism of chemical reactions. In this work, we report in situ tracking of bond breaking and making of an up-standing melamine molecule chemisorbed on Cu(100) by subnanometer resolved tip-enhanced Raman spectroscopy (TERS). We demonstrate a vertical detection depth of about 4 A with spectral sensitivity at the single chemical-bond level, which allows us not only to justify the up-standing configuration involving a dehydrogenation process at the bottom upon chemisorption, but also to specify the breaking of top N-H bonds and the transformation to its tautomer during photon-induced hydrogen transfer reactions. Our results indicate the chemical and structural sensitivity of TERS for single-molecule recognition beyond flat-lying planar molecules, providing new opportunities for probing the microscopic mechanism of molecular adsorption and surface reactions at the chemical-bond level.
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