Anomalous interfacial dynamics of single proton charges in binary aqueous solutions

Jean Comtet, Archith Rayabharam, Evgenii Glushkov, Miao Zhang, Ahmet Avsar, Kenji Watanabe, Takashi Taniguchi, Narayana R. Aluru, Aleksandra Radenovic

Research output: Contribution to journalArticlepeer-review

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.

Original languageEnglish (US)
Article numberabg8568
JournalScience Advances
Volume7
Issue number40
DOIs
StatePublished - Oct 2021

ASJC Scopus subject areas

  • General

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