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In high-resolution scanning probe microscopy, it is becoming increasingly common to simultaneously record multiple channels representing different tip-sample interactions to collect complementary information about the sample surface. A popular choice involves simultaneous scanning tunneling microscopy (STM) and noncontact atomic force microscopy (NC-AFM) measurements, which are thought to reflect the chemical and electronic properties of the sample surface. With surface-oxidized Cu(100) as an example, we investigate whether atomic-scale information on chemical interactions can be reliably extracted from frequency shift maps obtained while using the tunneling current as the feedback parameter. Ab initio calculations of interaction forces between specific tip apexes and the surface are utilized to compare experiments with theoretical expectations. The examination reveals that constant-current operation may induce a noticeable influence of topography-feedback-induced cross-talk on the frequency shift data, resulting in misleading interpretations of local chemical interactions on the surface. Consequently, the need to apply methods such as 3D-AFM is emphasized when accurate conclusions about both the local charge density near the Fermi level, as provided by the STM channel, and the site-specific strength of tip-sample interactions (NC-AFM channel) are desired. We conclude by generalizing to the case where multiple atomic-scale interactions are being probed while only one of them is kept constant. © 2015 American Chemical Society.
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A comprehensive analysis of contrast formation mechanisms in scanning tunneling microscopy (STM) experiments on a metal oxide surface is presented with the oxygen-induced (2√2×√2)R45 missing row reconstruction of the Cu(100) surface as a model system. Density functional theory and electronic transport calculations were combined to simulate the STM imaging behavior of pure and oxygen-contaminated metal tips with structurally and chemically different apexes while systematically varying bias voltage and tip-sample distance. The resulting multiparameter database of computed images was used to conduct an extensive comparison with experimental data. Excellent agreement was attained for a large number of cases, suggesting that the assumed model tips reproduce most of the commonly encountered contrast-determining effects. Specifically, we find that depending on the bias voltage polarity, copper-terminated tips allow selective imaging of two structurally distinct surface Cu sites, while oxygen-terminated tips show complex contrasts with pronounced asymmetry and tip-sample distance dependence. Considering the structural and chemical stability of the tips reveals that the copper-terminated apexes tend to react with surface oxygen at small tip-sample distances. In contrast, oxygen-terminated tips are considerably more stable, allowing exclusive surface oxygen imaging at small tip-sample distances. Our results provide a conclusive understanding of fundamental STM imaging mechanisms, thereby providing guidelines for experimentalists to achieve chemically selective imaging by properly selecting imaging parameters. © 2013 American Chemical Society.
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The influence of defects on the local structural, electronic, and chemical properties of a surface oxide on Cu(100) were investigated using atomic resolution three-dimensional force mapping combined with tunneling current measurements and ab initio density functional theory. Results reveal that the maximum attractive force between tip and sample occurs above the oxygen atoms; theory indicates that the tip, in this case, terminates in a Cu atom. Meanwhile, simultaneously acquired tunneling current images emphasize the positions of Cu atoms, thereby, providing species-selective contrast in the two complementary data channels. One immediate outcome is that defects due to the displacement of surface copper are exposed in the current maps, even though force maps only reflect a well-ordered oxygen sublattice. The exact nature of the defects is confirmed by the simulations, which also reveal that the arrangement of the oxygen atoms is not disrupted by the copper displacement. In addition, the experimental force maps uncover a position-dependent modulation of the attractive forces between the surface oxygen and the copper-terminated tips, which is found to reflect the surface's inhomogeneous chemical and structural environment. As a consequence, the demonstrated method has the potential to directly probe how defects affect surface chemical interactions. © 2013 American Physical Society.
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- Journal Article (3)