Nanoscale Topography Influences Polymer Surface Diffusion

Wang, Dapeng; He, Chunlin; Stoykovich, Mark P.; Schwartz, Daniel K.

doi:10.1021/nn506376n

Cited by 103 publications

(149 citation statements)

References 58 publications

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“…14 Similar slowing of Fickian diffusion coincident with non-Gaussian distributions of particle displacements has been observed in a variety of systems, including hard sphere colloidal dispersions, 15,16 polymers in an array of pillars, 17 nanoparticles in a porous polymer matrix, 18 and colloids in a matrix of entangled F-actin polymers. Thus particle diffusion typically becomes slower in confinement.…”

Section: Introductionmentioning

confidence: 55%

“…17,18,29,30 Using one class of micromodels that simulate natural porous media, arrays of micro-and nanoscale posts in silicon and glass microchannels, 14,31,32 earlier experiments examined weak to moderate confinements. 17,18,29,30 Using one class of micromodels that simulate natural porous media, arrays of micro-and nanoscale posts in silicon and glass microchannels, 14,31,32 earlier experiments examined weak to moderate confinements.…”

Section: Introductionmentioning

confidence: 99%

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Diffusive dynamics of nanoparticles in ultra-confined media

Jacob

Retterer

et al. 2015

Soft Matter

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Differential dynamic microscopy (DDM) was used to investigate the diffusive dynamics of nanoparticles of diameter 200-400 nm that were strongly confined in a periodic square array of cylindrical nanoposts. The minimum distance between posts was 1.3-5 times the diameter of the nanoparticles. The image structure functions obtained from the DDM analysis were isotropic and could be fit by a stretched exponential function. The relaxation time scaled diffusively across the range of wave vectors studied, and the corresponding scalar diffusivities decreased monotonically with increased confinement. The decrease in diffusivity could be described by models for hindered diffusion that accounted for steric restrictions and hydrodynamic interactions. The stretching exponent decreased linearly as the nanoparticles were increasingly confined by the posts. Together, these results are consistent with a picture in which strongly confined nanoparticles experience a heterogeneous spatial environment arising from hydrodynamics and volume exclusion on time scales comparable to cage escape, leading to multiple relaxation processes and Fickian but non-Gaussian diffusive dynamics.

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Section: Introductionmentioning

confidence: 55%

Section: Introductionmentioning

confidence: 99%

Diffusive dynamics of nanoparticles in ultra-confined media

Jacob

Retterer

et al. 2015

Soft Matter

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“…Diffusion of polymers 6 and peptides 7 is known to be slowed down near surfaces with nanoscopic roughness. Therefore, we were interested how cylinder-like objects with smooth versus rough surface influence the mobility of lipids and their acyl chains in membranes.…”

Section: Figurementioning

confidence: 99%

Roughness of a transmembrane peptide reduces lipid membrane dynamics

Olšinová

Jurkiewicz

Sýkora

et al. 2016

Preprint

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Transmembrane domains integrate proteins into cellular membranes and support their function. The capacity of these prevalently a-helical structures in mammals to influence membrane properties is poorly understood. Combining experiments with molecular dynamics simulations, we provide evidence that helical transmembrane peptides with their rough surface reduce lateral mobility of membrane constituents. The molecular mechanism involves trapping of lipid acyl chains on the rough surface and segregation of cholesterol from the vicinity of peptides. The observations are supported by our toy model indicating strong effect of rough objects on membrane dynamics. Herein described effect has implications for the organization and function of biological membranes, especially the plasma membrane with high cholesterol content.

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“…[24,[39][40][41][42][43]. The results presented here provide a comprehensive picture of how and why adsorbate-surface interactions influence interfacial motion.…”

Section: Prl 119 268001 (2017) P H Y S I C a L R E V I E W L E T T Ementioning

confidence: 77%

3D Imaging of Hopping Molecules

Barkai

Garini

2017

Physics

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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. DOI: 10.1103/PhysRevLett.119.268001 Molecular transport in fluid phases is understood in terms of the Brownian motion of individual molecules and particles, and can, therefore, be predicted and controlled by parameters including the hydrodynamic radius and fluid viscosity. In contrast, the analogous behavior at the interfaces remains poorly understood despite its fundamental interest and technological relevance; i.e., the dynamics of macromolecules at solid-liquid interfaces underlie many applications including chemical sensing, catalysis, lubrication, and adhesion [1][2][3][4][5][6]. While interfacial diffusion is nominally two dimensional (2D) and conventionally described in terms of 2D Brownian motion, longstanding theoretical models [7][8][9][10][11][12][13][14][15][16] have predicted that interfacial mass transport could actually be dominated by "flights" through an adjacent liquid phase, which would dramatically alter the nature of interfacial molecular motion; an understanding of this process is necessary in order to rationally control mass transport at surfaces. Recent experimental results indirectly support these predictions by measuring the 2D projection of trajectories for atoms, molecules, polymers, and nanoparticles, in thin films, at solid-liquid interface, and on lipid bilayers, which can be represented as an intermittent process with periods of apparent immobility alternating with long flights comprising a heavy-tailed distribution [17][18][19][20][21][22][23][24][25][26]. However, the evidence for the presence of three-dimensional (3D) hops remains indirect, and critical aspects of the proposed "hopping" process remain a mystery. For example, theoretical models represent a flight as a series of hops (i.e., ...

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Nanoscale Topography Influences Polymer Surface Diffusion

Cited by 103 publications

References 58 publications

Diffusive dynamics of nanoparticles in ultra-confined media

Diffusive dynamics of nanoparticles in ultra-confined media

Roughness of a transmembrane peptide reduces lipid membrane dynamics

3D Imaging of Hopping Molecules

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