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research article

Anomalous interfacial dynamics of single proton charges in binary aqueous solutions

Comtet, Jean  
•
Rayabharam, Archith
•
Glushkov, Evgenii  
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October 1, 2021
Science Advances

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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Type
research article
DOI
10.1126/sciadv.abg8568
Web of Science ID

WOS:000703091100010

Author(s)
Comtet, Jean  
Rayabharam, Archith
Glushkov, Evgenii  
Zhang, Miao  
Avsar, Ahmet
Watanabe, Kenji
Taniguchi, Takashi
Aluru, Narayana R.
Radenovic, Aleksandra  
Date Issued

2021-10-01

Publisher

AMER ASSOC ADVANCEMENT SCIENCE

Published in
Science Advances
Volume

7

Issue

40

Article Number

eabg8568

Subjects

Multidisciplinary Sciences

•

Science & Technology - Other Topics

•

total-energy calculations

•

molecular-dynamics

•

water

•

surface

•

membrane

•

localization

•

diffusion

•

transport

•

defects

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LBEN  
Available on Infoscience
October 23, 2021
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/182542
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