Theory of Transient Localization, Activated Dynamics, and a Macromolecular Glass Transition in Ring Polymer Liquids

Published on Oct 19, 2021in ACS Macro Letters6.903
· DOI :10.1021/ACSMACROLETT.1C00530
Baicheng Mei5
Estimated H-index: 5
,
Zachary E. Dell6
Estimated H-index: 6
,
Kenneth S. Schweizer80
Estimated H-index: 80
Source
Abstract
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References47
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#1Margarita Kruteva (Forschungszentrum J√ľlich)H-Index: 7
#2J√ľrgen Allgaier (Forschungszentrum J√ľlich)H-Index: 31
Last. Dieter Richter (Forschungszentrum J√ľlich)H-Index: 75
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We report a comprehensive study on the molecular conformation and dynamics of very large poly(ethylene oxide) rings in the melt: (i) for all rings, independent of the ring size, by small angle neutron scattering we observe a crossover from a strong Q-dependence at intermediate Q to a Q ‚ąí 2 dependence at higher Q. Constructing a generic model including a crossover from Gaussian statistics at short distances to more compact structures at larger distances, we find the crossover at a distance along ...
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#1Ashesh Ghosh (UIUC: University of Illinois at Urbana‚ÄďChampaign)H-Index: 4
We theoretically study the effect of external deformation on activated structural relaxation and aspects of the nonlinear mechanical response of glassy hard sphere fluids in the context of elastically collective nonlinear Langevin equation theory. This microscopic force-based approach describes activated relaxation as a coupled local-nonlocal event involving caging and longer range collective elasticity, with the latter becoming more important and ultimately dominant with increasing packing frac...
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#1Baicheng Mei (UIUC: University of Illinois at Urbana‚ÄďChampaign)H-Index: 5
#2Zachary E. Dell (UIUC: University of Illinois at Urbana‚ÄďChampaign)H-Index: 6
Last. Kenneth S. SchweizerH-Index: 80
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We construct a microscopic theory at the level of segment-scale correlated space‚Äďtime intermolecular forces for the long-time center-of-mass (CM) diffusion constant and intermediate-time non-Fickia...
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#1Baicheng MeiH-Index: 5
#2Yuxing ZhouH-Index: 8
Last. Kenneth S. Schweizer (UIUC: University of Illinois at Urbana‚ÄďChampaign)H-Index: 80
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We employ the microscopic Elastically Collective Nonlinear Langevin Equation (ECNLE) theory of activated dynamics in combination with crystal-avoiding simulations to study four inter-related questi...
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#1Jan Smrek (University of Vienna)H-Index: 10
#2Iurii Chubak (University of Vienna)H-Index: 6
Last. Kurt Kremer (MPG: Max Planck Society)H-Index: 94
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The glass transition in soft matter systems is generally triggered by an increase in packing fraction or a decrease in temperature. It has been conjectured that the internal topology of the constituent particles, such as polymers, can cause glassiness too. However, the conjecture relies on immobilizing a fraction of the particles and is therefore difficult to fulfill experimentally. Here we show that in dense solutions of circular polymers containing (active) segments of increased mobility, the ...
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#1Kenneth S. Schweizer (UIUC: University of Illinois at Urbana‚ÄďChampaign)H-Index: 80
#2David S. Simmons (USF: University of South Florida)H-Index: 20
The nature of alterations to dynamics and vitrification in the nanoscale vicinity of interfaces‚ÄĒcommonly referred to as ‚Äúnanoconfinement‚ÄĚ effects on the glass transition‚ÄĒhas been an open question for a quarter century. We first analyze experimental and simulation results over the last decade to construct an overall phenomenological picture. Key features include the following: after a metrology- and chemistry-dependent onset, near-interface relaxation times obey a fractional power law decoupling ...
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#1Julian Oberdisse (University of Montpellier)H-Index: 32
#2Marina Gonz√°lez-Burgos (CSIC: Spanish National Research Council)H-Index: 7
Last. Juan Colmenero (Donostia International Physics Center)H-Index: 73
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The conformation of single-chain nanoparticles (SCNPs) in the presence of linear polystyrene crowding molecules has been studied by small-angle neutron scattering under contrast-matching of the crowders. A model describing the scattering of aggregating polydisperse SCNPs has been developed, resulting in the determination of the potentially squeezed size of the individual SCNPs within aggregates, their local chain statistics, and the average aggregation number, as a function of crowding. Two diff...
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#1Zachary E. Dell (UMass: University of Massachusetts Amherst)H-Index: 6
We employ the field theoretic polymer integral equation theory to construct a segment-level theory for the thermodynamics and pair structure of dense liquids of interpenetrating ring polymers and a simple globule model. The latter is defined by a fractal mass distribution on all internal length scales with an exponent equal to the spatial dimension (dF = ds = 3). In an isochoric ensemble the dimensionless compressibility and pressure is predicted to vary exponentially with macromolecular volume ...
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Motivated by recent observations that non-concatenated ring polymers in their dense solution exhibit a glass-like dynamics, we propose a free volume description of the motion of such rings based on the notion of topological volume. We first construct a phenomenological free energy which enables one to qnaitify the degree of topological crowding measured by the coordination number. Then we pinpoint a key role of the cooperative dynamics of neighboring rings, which is responsible for an anomalous ...
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#1Takahiro Sakaue (Aoyama Gakuin University)H-Index: 25
Motivated by recent observations that non-concatenated ring polymers in their dense solution exhibit a glass-like dynamics, we propose a free volume description of the motion of such rings based on the notion of topological volume. We first construct a phenomenological free energy which enables one to quantify the degree of topological crowding measured by the coordination number. Then we pinpoint a key role of the cooperative dynamics of neighboring rings, which is responsible for an anomalous ...
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