In-situ nanospectroscopic imaging of plasmon-induced two-dimensional [4+4]-cycloaddition polymerization on Au(111).
AuthorsShao, Feng; orcid: 0000-0003-3879-5884; email: email@example.com
Zhang, Yao; orcid: 0000-0002-6524-0289
Lan, Jinggang; email: firstname.lastname@example.org
Dieter Schlüter, A
Zenobi, Renato; orcid: 0000-0001-5211-4358; email: email@example.com
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AbstractPlasmon-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.
CitationNature communications, volume 12, issue 1, page 4557
DescriptionFrom Europe PMC via Jisc Publications Router
History: ppub 2021-07-01, epub 2021-07-27
Publication status: Published
Funder: European Research Council; Grant(s): 741431-2DNanoSpec, 741431
Funder: Swiss National Science Foundation; Grant(s): URPP-LightChEC
Funder: EC | Horizon 2020 Framework Programme (EU Framework Programme for Research and Innovation H2020); Grant(s): 841653-2DvdWHs