Simultaneous Measurement of Multiple Independent Atomic-Scale Interactions Using Scanning Probe Microscopy: Data Interpretation and the Effect of Cross-Talk

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.