Here we report the bias-evolution of the electrical double layer structure of an ionic liquid on highly ordered pyrolytic graphite measured by atomic force microscopy. We observe reconfiguration under applied bias and the orientational transitions in the Stern layer. The synergy between molecular dynamics simulation and experiment provides a comprehensive picture of structural phenomena and long and short-range interactions, which improves our understanding of the mechanism of charge storage on a molecular level.

Tapping mode atomic force microscopy (AFM), also known as amplitude modulated (AM) or AC mode, is a proven, reliable and gentle imaging mode with widespread applications. Over the several decades that tapping mode has been in use, quantification of tip-sample mechanical properties such as stiffness has remained elusive. Bimodal tapping mode keeps the advantages of single-frequency tapping mode while extending the technique by driving and measuring an

SummaryBimodal atomic force microscopy uses a cantilever that is simultaneously driven at two of its eigenmodes (resonant modes). Parameters associated with both resonances can be measured and used to extract quantitative nanomechanical information about the sample surface. Driving the first eigenmode at a large amplitude and a higher eigenmode at a small amplitude simultaneously provides four independent observables that are sensitive to the tip–sample nanomechanical interaction parameters. To demonstrate this, a generalized theoretical framework for extracting nanomechanical sample properties from bimodal experiments is presented based on Hertzian contact mechanics. Three modes of operation for measuring cantilever parameters are considered: amplitude, phase, and frequency modulation. The experimental equivalence of all three modes is demonstrated on measurements of the second eigenmode parameters. The contact mechanics theory is then extended to power-law tip shape geometries, which is applied to analyze the experimental data and extract a shape and size of the tip interacting with a polystyrene surface.

An ongoing challenge in atomic force microscope (AFM) experiments is the quantitative measurement of cantilever motion. The vast majority of AFMs use the optical beam deflection (OBD) method to infer the deflection of the cantilever. The OBD method is easy to implement, has impressive noise performance and tends to be mechanically robust. However, it represents an indirect measurement of the cantilever displacement, since it is fundamentally an angular rather than a displacement measurement. Here, we demonstrate a metrological AFM that combines an OBD sensor with a laser Doppler vibrometer (LDV) to enable accurate measurements of the cantilever velocity and displacement. The OBD/LDV AFM allows a host of quantitative measurements to be performed, including in-situ measurements of cantilever oscillation modes in piezoresponse force microscopy (PFM). As an example application, we demonstrate how this instrument can be used for accurate quantification of piezoelectric sensitivity -a longstanding goal in the electromechanical community.

In attempting to perform frequency modulation atomic force microscopy (FM-AFM) in liquids, a non-flat phase transfer function in the self-excitation system prevents proper tracking of the cantilever natural frequency. This results in frequency-and-phase modulation atomic force microscopy (FPM-AFM) which lies in between phase modulation atomic force microscopy (PM-AFM) and FM-AFM. We derive the theory necessary to recover the conservative force and damping in such a situation, where standard FM-AFM theory no longer applies. Although our recovery procedure applies to all cantilever excitation methods in principle, its practical implementation may be difficult, or even impossible, if the cantilever is driven piezoacoustically. Specifically, we contrast the piezoacoustic excitation method to the photothermal method in the context of force spectroscopy of hydration structures at the mica-water interface. The results clearly demonstrate that photothermal excitation is superior to piezoacoustic excitation, as it allows for accurate quantitative interpretation of the acquired data