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Anomalous interfacial dynamics of single proton charges in binary aqueous solutions

Abstract : Our understanding of the dynamics of charge transfer between solid surfaces and liquid electrolytes has been hampered by the difficulties in obtaining interface, charge, and solvent-specific information at both high spatial and temporal resolution. Here, we measure at the single charge scale the dynamics of protons at the interface between an hBN crystal and binary mixtures of water and organic amphiphilic solvents (alcohols and acetone), evidencing a marked influence of solvation on interfacial dynamics. Applying single-molecule localization microscopy to emissive crystal defects, we observe correlated activation between adjacent ionizable surface defects, mediated by the transport of single excess protons along the solid/liquid interface. Solvent content has a nontrivial effect on interfacial dynamics, leading at intermediate water fraction to an increased surface diffusivity, as well as an increased affinity of the proton charges to the solid surface. Our measurements evidence the notable role of solvation on interfacial proton charge transport.
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Submitted on : Thursday, September 30, 2021 - 4:43:31 PM
Last modification on : Wednesday, May 11, 2022 - 10:00:05 AM
Long-term archiving on: : Friday, December 31, 2021 - 9:13:39 PM



Jean Comtet, Archith Rayabharam, Evgenii Glushkov, Miao Zhang, Avsar Ahmet, et al.. Anomalous interfacial dynamics of single proton charges in binary aqueous solutions. Science Advances , American Association for the Advancement of Science (AAAS), 2021, 7 (40), ⟨10.1021/acsnano.1c00373⟩. ⟨hal-03360245⟩



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