Journal
PHYSICAL REVIEW LETTERS
Volume 119, Issue 26, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.119.268001
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Funding
- U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0001854]
- Chinese The Thousand Talents Plan for Young Professionals
- International Science and Technology Cooperation Program of Jilin, China
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Theoretical predictions have suggested that molecular motion at interfaces-which influences processes including heterogeneous catalysis, (bio) chemical sensing, lubrication and adhesion, and nanomaterial self-assembly-may be dominated by hypothetical hops through the adjacent liquid phase, where a diffusing molecule readsorbs after a given hop according to a probabilistic sticking coefficient. Here, we use three-dimensional (3D) single-molecule tracking to explicitly visualize this process for human serum albumin at solid-liquid interfaces that exert varying electrostatic interactions on the biomacromolecule. Following desorption from the interface, a molecule experiences multiple unproductive surface encounters before readsorption. An average of approximately seven surface collisions is required for the repulsive surfaces, decreasing to approximately two and a half for surfaces that are more attractive. The hops themselves are also influenced by long-range interactions, with increased electrostatic repulsion causing hops of longer duration and distance. These findings explicitly demonstrate that interfacial diffusion is dominated by biased 3D Brownian motion involving bulk-surface coupling and that it can be controlled by influencing short- and long-range adsorbate-surface interactions.
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