Cargando…
Anomalous interfacial dynamics of single proton charges in binary aqueous solutions
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 dyn...
Autores principales: | , , , , , , , , |
---|---|
Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Association for the Advancement of Science
2021
|
Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8480921/ https://www.ncbi.nlm.nih.gov/pubmed/34586851 http://dx.doi.org/10.1126/sciadv.abg8568 |
_version_ | 1784576571528445952 |
---|---|
author | Comtet, Jean Rayabharam, Archith Glushkov, Evgenii Zhang, Miao Avsar, Ahmet Watanabe, Kenji Taniguchi, Takashi Aluru, Narayana R. Radenovic, Aleksandra |
author_facet | Comtet, Jean Rayabharam, Archith Glushkov, Evgenii Zhang, Miao Avsar, Ahmet Watanabe, Kenji Taniguchi, Takashi Aluru, Narayana R. Radenovic, Aleksandra |
author_sort | Comtet, Jean |
collection | PubMed |
description | 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. |
format | Online Article Text |
id | pubmed-8480921 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2021 |
publisher | American Association for the Advancement of Science |
record_format | MEDLINE/PubMed |
spelling | pubmed-84809212021-10-08 Anomalous interfacial dynamics of single proton charges in binary aqueous solutions Comtet, Jean Rayabharam, Archith Glushkov, Evgenii Zhang, Miao Avsar, Ahmet Watanabe, Kenji Taniguchi, Takashi Aluru, Narayana R. Radenovic, Aleksandra Sci Adv Physical and Materials Sciences 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. American Association for the Advancement of Science 2021-09-29 /pmc/articles/PMC8480921/ /pubmed/34586851 http://dx.doi.org/10.1126/sciadv.abg8568 Text en Copyright © 2021 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC). https://creativecommons.org/licenses/by-nc/4.0/This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license (https://creativecommons.org/licenses/by-nc/4.0/) , which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited. |
spellingShingle | Physical and Materials Sciences Comtet, Jean Rayabharam, Archith Glushkov, Evgenii Zhang, Miao Avsar, Ahmet Watanabe, Kenji Taniguchi, Takashi Aluru, Narayana R. Radenovic, Aleksandra Anomalous interfacial dynamics of single proton charges in binary aqueous solutions |
title | Anomalous interfacial dynamics of single proton charges in binary aqueous solutions |
title_full | Anomalous interfacial dynamics of single proton charges in binary aqueous solutions |
title_fullStr | Anomalous interfacial dynamics of single proton charges in binary aqueous solutions |
title_full_unstemmed | Anomalous interfacial dynamics of single proton charges in binary aqueous solutions |
title_short | Anomalous interfacial dynamics of single proton charges in binary aqueous solutions |
title_sort | anomalous interfacial dynamics of single proton charges in binary aqueous solutions |
topic | Physical and Materials Sciences |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8480921/ https://www.ncbi.nlm.nih.gov/pubmed/34586851 http://dx.doi.org/10.1126/sciadv.abg8568 |
work_keys_str_mv | AT comtetjean anomalousinterfacialdynamicsofsingleprotonchargesinbinaryaqueoussolutions AT rayabharamarchith anomalousinterfacialdynamicsofsingleprotonchargesinbinaryaqueoussolutions AT glushkovevgenii anomalousinterfacialdynamicsofsingleprotonchargesinbinaryaqueoussolutions AT zhangmiao anomalousinterfacialdynamicsofsingleprotonchargesinbinaryaqueoussolutions AT avsarahmet anomalousinterfacialdynamicsofsingleprotonchargesinbinaryaqueoussolutions AT watanabekenji anomalousinterfacialdynamicsofsingleprotonchargesinbinaryaqueoussolutions AT taniguchitakashi anomalousinterfacialdynamicsofsingleprotonchargesinbinaryaqueoussolutions AT alurunarayanar anomalousinterfacialdynamicsofsingleprotonchargesinbinaryaqueoussolutions AT radenovicaleksandra anomalousinterfacialdynamicsofsingleprotonchargesinbinaryaqueoussolutions |