Journal
MACROMOLECULES
Volume 53, Issue 10, Pages 4110-4120Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.macromol.9b02365
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Funding
- U.S. Department of Energy, Office of Science, Basic Energy Sciences [DESC0001854]
- U.S. Defense Threat Reduction Agency [HDTRA116-1-0045]
- Soft Materials Research Center [NSF-MRSEC DMR 1420736]
- NIST-CU Cooperative Agreement [70NANB15H226]
- NIH/CU Molecular Biophysics Graduate Traineeship [T32 GM065103]
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The surface diffusion of poly-L-lysine (PLL) in a planar nanoslit was studied using convex lens-induced confinement (CLiC) single-molecule tracking microscopy. Three surface chemistries were employed to understand the interplay of electrostatic and short-range interactions: an amine-functionalized silica surface, an oligo(ethylene oxide) (OEG)-modified surface, and a 1:1 mixture of the two ligands. Effective surface diffusion coefficients increased rapidly with slit height until saturating for slit heights <30 nm. While diffusion at a semi-infinite interface was significantly faster for OEG surfaces, the diffusion coefficient increased most rapidly with slit height for amine-functionalized surfaces, resulting in surface diffusion within very thin slits being nearly independent of surface chemistry. Intermittent random walks were simulated within a planar slit geometry, using experimentally measured parameters obtained from diffusion at a single interface to account for the characteristic short-range interactions between PLL and each surface chemistry, and were in good agreement with experimental measurements.
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