Multiscale Imaging Methodology for Surface Morphological Changes in Lithium Metal Anode Using Coupled Operando OM and In Situ EC‐AFM

ABSTRACT Microscopy techniques are widely employed to confirm the effectiveness of electrodes and electrolytes designed to suppress dendrites in lithium metal anodes. Although optical microscopy (OM) and atomic force microscopy (AFM) are widely used, they are typically performed in isolation, preventing correlative analysis of the same regions. Moreover, OM suffers from limited spatial resolution, whereas AFM affords only localized insights. Thus, an integrated methodology combining operando OM and in situ electrochemical AFM (EC‐AFM) was invented for surface characterization of the lithium metal anode in lithium/lithium symmetric cells under 0.5 and 3 mA cm ⁻² . OM visualizes microscale features such as dendrites, pit formation, and surface darkening during stripping, while EC‐AFM resolves nanoscale structures at the same darkened sites, unattainable by OM. This multiscale approach enables a qualitative and quantitative comparison of surface evolution, overcoming the individual limitations of each microscopy method and providing an analysis methodology that is expandable for evaluating other electrodes and electrolytes.