Dynamics of Nanoparticles in Entangled Polymer Solutions

Nath, Pooja; Mangal, Rahul; Kohle, Ferdinand; Choudhury, Snehashis; Narayanan, Suresh; Wiesner, Ulrich; Archer, Lynden A.

doi:10.1021/acs.langmuir.7b03418

Dynamics of Nanoparticles in Entangled Polymer Solutions

Journal Article · Fri Dec 01 00:00:00 EST 2017 · Langmuir

DOI:https://doi.org/10.1021/acs.langmuir.7b03418· OSTI ID:1421961

Nath, Pooja ^[1]; Mangal, Rahul ^[2]; Kohle, Ferdinand ^[1]; Choudhury, Snehashis ^[1]; Narayanan, Suresh ^[3]; ^[1]; ^[1]

Cornell Univ., Ithaca, NY (United States)
Cornell Univ., Ithaca, NY (United States); Indian Institute of Technology Kanpur, Uttar Pradesh (India)
Argonne National Lab. (ANL), Argonne, IL (United States)

The mean square displacement < r² > of nanoparticle probes dispersed in simple isotropic liquids and in polymer solutions is interrogated using fluorescence correlation spectroscopy and single-particle tracking (SPT) experiments. Probe dynamics in different regimes of particle diameter (d), relative to characteristic polymer length scales, including the correlation length (ξ), the entanglement mesh size (a), and the radius of gyration (R_g), are investigated. In simple fluids and for polymer solutions in which d >> R_g, long-time particle dynamics obey random-walk statistics < r² >:t, with the bulk zero-shear viscosity of the polymer solution determining the frictional resistance to particle motion. In contrast, in polymer solutions with d < R_g, polymer molecules in solution exert noncontinuum resistances to particle motion and nanoparticle probes appear to interact hydrodynamically only with a local fluid medium with effective drag comparable to that of a solution of polymer chain segments with sizes similar to those of the nanoparticle probes. Under these conditions, the nanoparticles exhibit orders of magnitude faster dynamics than those expected from continuum predictions based on the Stokes–Einstein relation. SPT measurements further show that when d > a, nanoparticle dynamics transition from diffusive to subdiffusive on long timescales, reminiscent of particle transport in a field with obstructions. This last finding is in stark contrast to the nanoparticle dynamics observed in entangled polymer melts, where X-ray photon correlation spectroscopy measurements reveal faster but hyperdiffusive dynamics. As a result, we analyze these results with the help of the hopping model for particle dynamics in polymers proposed by Cai et al. and, on that basis, discuss the physical origins of the local drag experienced by the nanoparticles in entangled polymer solutions.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1421961

Journal Information:: Langmuir, Journal Name: Langmuir Journal Issue: 1 Vol. 34; ISSN 0743-7463

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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