Optical nanoscopy of spatiotemporal metal stripping cooperativity at single-ion and subparticle resolution

Coupled ion-electron interfacial reactivities on electroactive particles are complex and crucial to various battery chemistries and dynamics, yet direct visualization of these reactions remains elusive despite advances in operando imaging. Here we report ion-localization optical nanoscopy (ION) with single-ion, subparticle resolution that distinguishes microscopic static and dynamic disorder in ion-generation interfacial reactivity, offering nondestructive, real-time, non-equilibrium insights. We uncover diverse stripping dynamics of zinc anodes, revealing unexpected subparticle-level heterogeneity and challenging conventional views of uniform stripping on (002)-textured zinc. Mesoscale functional descriptors-intraparticle diffusive and electronic coupling strengths-that govern overall stripping uniformity are identified by ION, supported by computational methods and validated by in situ single-particle manipulation. Imaging-derived insights are further translated into ensemble-level strategies enabling exceptional anode reversibility. ION is cost-effective, high-throughput and broadly applicable to myriad ion-participated interfacial processes, including cathode (de)intercalation, solid-electrolyte interphase evolution, ion exchange and catalyst restructuring.