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In-situ nanospectroscopic imaging of plasmon-induced two-dimensional [4+4]-cycloaddition polymerization on Au(111).
Shao, Feng; Wang, Wei; Yang, Weimin; Yang, Zhilin; Zhang, Yao; Lan, Jinggang; Dieter Schlüter, A; Zenobi, Renato.
Afiliación
  • Shao F; Department of Physics and Astronomy, National Graphene Institute, University of Manchester, Manchester, UK. feng.shao@manchester.ac.uk.
  • Wang W; Department of Chemistry and Applied Biosciences, ETH Zurich, Zurich, Switzerland. feng.shao@manchester.ac.uk.
  • Yang W; Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, Chang-Kung Chuang Institute, East China Normal University, Shanghai, People's Republic of China.
  • Yang Z; Department of Physics, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Jiujiang Research Institute, Xiamen University, Xiamen, Fujian, People's Republic of China.
  • Zhang Y; Department of Physics, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Jiujiang Research Institute, Xiamen University, Xiamen, Fujian, People's Republic of China.
  • Lan J; Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, People's Republic of China.
  • Dieter Schlüter A; Department of Chemistry, University of Zurich, Zurich, Switzerland. jinggang.lan@chem.uzh.ch.
  • Zenobi R; Department of Materials, Polymer Chemistry, ETH Zurich, Zurich, Switzerland.
Nat Commun ; 12(1): 4557, 2021 Jul 27.
Article en En | MEDLINE | ID: mdl-34315909
Plasmon-induced chemical reactions (PICRs) have recently become promising approaches for highly efficient light-chemical energy conversion. However, an in-depth understanding of their mechanisms at the nanoscale still remains challenging. Here, we present an in-situ investigation by tip-enhanced Raman spectroscopy (TERS) imaging of the plasmon-induced [4+4]-cycloaddition polymerization within anthracene-based monomer monolayers physisorbed on Au(111), and complement the experimental results with density functional theory (DFT) calculations. This two-dimensional (2D) polymerization can be flexibly triggered and manipulated by the hot carriers, and be monitored simultaneously by TERS in real time and space. TERS imaging provides direct evidence for covalent bond formation with ca. 3.7 nm spatial resolution under ambient conditions. Combined with DFT calculations, the TERS results demonstrate that the lateral polymerization on Au(111) occurs by a hot electron tunneling mechanism, and crosslinks form via a self-stimulating growth mechanism. We show that TERS is promising to be plasmon-induced nanolithography for organic 2D materials.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2021 Tipo del documento: Article Pais de publicación: Reino Unido

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2021 Tipo del documento: Article Pais de publicación: Reino Unido