Anomalous interfacial dynamics of single proton charges in binary aqueous solutions

摘要: Understanding the dynamics of charge exchange between a solid surface and liquid is fundamental to various situations, ranging from nanofiltration catalysis electrochemistry. Charge transfer ultimately determined by physicochemical processes (surface group dissociation, ion adsorption, etc...) occurring in few layers molecules at interface liquid. Unfortunately, these remain largely uncharted due experimental challenges probing interfacial with sufficiently high spatial temporal resolution. Here, we resolve single-charge scale, proton charges an hBN crystal binary mixtures water organic amphiphilic solvents (e.g. alcohol), evidencing dramatic influence solvation on dynamics. Our observations rely application spectral Single Molecule Localization Microscopy (sSMLM) two types optically active defects surface, which act as intrinsic optical markers for both protonation interaction apolar alkyl groups solvent. We use sSMLM reveal transport succession jumps titratable defects, mediated solvated along solid/liquid interface. By changing relative concentration mixtures, evidence non-trivial effect dynamics, leading intermediate increased affinity accompanied diffusivity. These measurements confirm strong role establish potential single-molecule localization techniques probe wide range dynamic interfaces.