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Understanding the dynamics of charge exchange between a solid surface and aliquid is fundamental to various situations, ranging from nanofiltration tocatalysis and electrochemistry. Charge transfer is ultimately determined byphysicochemical processes (surface group dissociation, ion adsorption, etc...)occurring in the few layers of molecules at the interface between the solid andthe liquid. Unfortunately, these processes remain largely uncharted due to theexperimental challenges in probing interfacial charge dynamics withsufficiently high spatial and temporal resolution. Here, we resolve at thesingle-charge scale, the dynamics of proton charges at the interface between anhBN crystal and binary mixtures of water and organic amphiphilic solvents (e.g.alcohol), evidencing a dramatic influence of solvation on interfacial dynamics.Our observations rely on the application of spectral Single MoleculeLocalization Microscopy (sSMLM) to two types of optically active defects at thehBN surface, which act as intrinsic optical markers for both surfaceprotonation and interaction with apolar alkyl groups of the organic solvent. Weuse sSMLM to reveal interfacial proton charge transport as a succession ofjumps between the titratable surface defects, mediated by the transport of thesolvated proton charge along the solid/liquid interface. By changing therelative concentration of water in binary mixtures, we evidence a non-trivialeffect on interfacial proton charge dynamics, leading at intermediate waterconcentration to an increased affinity of the proton charge to the solidsurface, accompanied by an increased surface diffusivity. These measurementsconfirm the strong role of solvation on interfacial proton charge transport andestablish the potential of single-molecule localization techniques to probe awide range of dynamic processes at solid/liquid interfaces.

Anomalous interfacial dynamics of single proton charges in binary aqueous solutions