Contact
    Start Publications In-situ nanospectroscopic imaging of plasmon-induced ...
    ←  Publication Finder
    KSV NIMA

    In-situ nanospectroscopic imaging of plasmon-induced two-dimensional [4+4]-cycloaddition polymerization on Au(111)

    Year: 2021

    Journal: Nat. Commun., Volume 12, JUL 27

    Authors: Shao, Feng; Wang, Wei; Yang, Weimin; Yang, Zhilin; Zhang, Yao; Lan, Jinggang; Schlueter, A. Dieter; Zenobi, Renato

    Organizations: Marie-Sklodowska-Curie Individual Fellowship [841653-2]; European Research Council (ERC) [7414312]; Swiss National Science Foundation (SNSF); University Research Priority Program (URPP); Swiss National Supercomputing Centre (CSCS) [uzh1, s965]

    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.
    View publication