TY - JOUR
T1 - Anomalous interfacial dynamics of single proton charges in binary aqueous solutions
AU - Comtet, Jean
AU - Rayabharam, Archith
AU - Glushkov, Evgenii
AU - Zhang, Miao
AU - Avsar, Ahmet
AU - Watanabe, Kenji
AU - Taniguchi, Takashi
AU - Aluru, Narayana R.
AU - Radenovic, Aleksandra
N1 - Publisher Copyright:
© 2021 The Authors.
PY - 2021/10
Y1 - 2021/10
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85116319379&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85116319379&partnerID=8YFLogxK
U2 - 10.1126/sciadv.abg8568
DO - 10.1126/sciadv.abg8568
M3 - Article
C2 - 34586851
AN - SCOPUS:85116319379
SN - 2375-2548
VL - 7
JO - Science Advances
JF - Science Advances
IS - 40
M1 - abg8568
ER -