Research Article

Determining structural and chemical heterogeneities of surface species at the single-bond limit

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Science  19 Feb 2021:
Vol. 371, Issue 6531, pp. 818-822
DOI: 10.1126/science.abd1827

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Joint strategy for surface chemistry

Recent advances in the development of tip-based microscopy have led to angstrom-scale spatial resolution, but no technique provides univocal characterization of the structural and chemical heterogeneities of surface species. Using a model system of pentacene derivatives on the Ag(110) surface, Xu et al. show that the combination of scanning tunneling microscopy, atomic force microscopy, and tip-enhanced Raman scattering provides the electronic, structural, and chemical information sufficiently correlated for an unambiguous characterization of the different—but structurally similar—chemical species and their interaction with the metal surface with single-bond resolution. The proposed multitechnique approach could find wide application in fundamental studies of heterogeneous catalysis and surface chemistry in general.

Science, this issue p. 818


The structure determination of surface species has long been a challenge because of their rich chemical heterogeneities. Modern tip-based microscopic techniques can resolve heterogeneities from their distinct electronic, geometric, and vibrational properties at the single-molecule level but with limited interpretation from each. Here, we combined scanning tunneling microscopy (STM), noncontact atomic force microscopy (AFM), and tip-enhanced Raman scattering (TERS) to characterize an assumed inactive system, pentacene on the Ag(110) surface. This enabled us to unambiguously correlate the structural and chemical heterogeneities of three pentacene-derivative species through specific carbon-hydrogen bond breaking. The joint STM-AFM-TERS strategy provides a comprehensive solution for determining chemical structures that are widely present in surface catalysis, on-surface synthesis, and two-dimensional materials.

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