AbstractDeconvoluting the vibrations and harmonics in solid‐solid interfaces is crucial for designing materials with improved performance, durability, and functionality. The measured vibrating microcantilever signal in the dynamic atomic force microscopy (AFM) encompasses a multitude of distinct signatures reflecting a diverse array of material properties. Nevertheless, uncertainties persist in decoding these signatures, primarily arising from the interplay between attractive and repulsive forces. Consequently, it is challenging to correlate the generated harmonics within the solid‐solid interfaces with the imaged phase and topography of materials, as well as the occasional observed contrast reversal. In this study, the vibration harmonics produced at solid‐solid interfaces are correlated, linking them to short‐range nano‐mechanical characteristics through a comprehensive blend of theory, simulation, and experimental methods. These findings shed light on the roots of harmonic generation and contrast reversals, opening avenues for designing innovative materials with customized properties.
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