Multiscale Functional Imaging of Interfaces through Atomic Force Microscopy Using Harmonic Mixing

The spatial resolution of atomic force microscopy (AFM) needed to resolve material interfaces is limited by the tip-sample separation ( d) dependence of the force used to record an image. Here, we present a new multiscale functional imaging technique that allows for in situ tunable spatial resolution, which can be applied to a wide range of inhomogeneous materials, devices, and interfaces. Our approach uses a multifrequency method to generate a signal whose d-dependence is controlled by mixing harmonics of the cantilever's oscillation with a modulated force. The spatial resolution of the resulting image is determined by the signal's d-dependence. Our measurements using harmonic mixing (HM) show that we can change the d-dependence of a force signal to improve spatial resolution by up to a factor of two compared to conventional methods. We demonstrate the technique with both Kelvin probe force microscopy (KPFM) and bimodal AFM to show its generality. Bimodal AFM with harmonic mixing actuation separates conservative from dissipative forces and is used to identify the regions of adhesive residue on exfoliated graphene. Our electrostatic measurements with open-loop KPFM demonstrate that multiple force modulations may be applied at once. Further, this method can be applied to any tip-sample force that can be modulated, for example, electrostatic, magnetic, and photoinduced forces, showing its universality. Because HM enables in situ switching between high sensitivity and high spatial resolution with any periodic driving force, we foresee this technique as a critical advancement for multiscale functional imaging.