Temporally Anticorrelated Subdiffusion in Water Nanofilms on Silica Suggests Near-Surface Viscoelasticity

Sarfati, Raphaël; Schwartz, Daniel K.

doi:10.1021/acsnano.9b07910

Temporally Anticorrelated Subdiffusion in Water Nanofilms on Silica Suggests Near-Surface Viscoelasticity

Journal Article · Tue Jan 14 00:00:00 EST 2020 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.9b07910· OSTI ID:1773884

^[1]; Schwartz, Daniel K. ^[2]

Univ. of Colorado, Boulder, CO (United States); University of Colorado Boulder
Univ. of Colorado, Boulder, CO (United States)

Here, single-molecule tracking was used to probe the local rheology of interfacial water. Fluorescent rhodamine molecules were tracked on silica surfaces as a function of ambient relative humidity, which controlled the thickness of condensed water nanofilms. At low humidity, the molecules exhibited confined diffusion in the vicinity of isolated adsorption sites characterized by a broad distribution of binding stiffness constants; subsequent chemical or physical surface passivation selectively eliminated stiffer binding sites. At increased humidity, molecularly thin water films condensed, permitting near-surface transport of rhodamine molecules. Motion was subdiffusive, with an anomalous exponent increasing with the nanofilm thickness. Molecular trajectories were temporally anticorrelated, ergodic, but also featured transient binding and intermittent diffusion. Statistical modeling demonstrated that this complex motion in water nanofilms had the characteristics of fractional Brownian motion combined with a continuous-time random walk. This was consistent with diffusion within viscoelastic nanofilms, suggesting persistent molecular structuring in the vicinity of the silica surface.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Colorado, Boulder, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001854

OSTI ID:: 1773884

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 3 Vol. 14; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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confined diffusion
silica
single-molecule tracking
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Temporally Anticorrelated Subdiffusion in Water Nanofilms on Silica Suggests Near-Surface Viscoelasticity

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