Dynamics of Shape-Persistent Giant Molecules: Zimm-like Melt, Elastic Plateau, and Cooperative Glass-like

Liu, GengXin; Feng, Xueyan; Lang, Kening; Zhang, Ruimeng; Guo, Dong; Yang, Shuguang; Cheng, Stephen Z.  D.

doi:10.1021/acs.macromol.7b01058

Title: Dynamics of Shape-Persistent Giant Molecules: Zimm-like Melt, Elastic Plateau, and Cooperative Glass-like

Journal Article · Thu Aug 31 00:00:00 EDT 2017 · Macromolecules

DOI:https://doi.org/10.1021/acs.macromol.7b01058· OSTI ID:1406629

^[1]; Feng, Xueyan ^[1]; Lang, Kening ^[1]; Zhang, Ruimeng ^[1]; Guo, Dong ^[1]; Yang, Shuguang ^[2];

^[1]

Univ. of Akron, OH (United States)
Donghua Univ., Shanghai (China)

Giant molecules are a new class of soft matter having threedimensional (3D) shapes and composed of chemically linked rigid molecular nanoparticles. Structurally, a 3D cluster of molecular nanoparticles can be one giant molecule or a few giant molecules associated together via specific interactions. The dynamics of clusters that are smaller than a critical diameter (~5 nm) presents a power law relaxation exponent of 0.7 at the high frequency region corresponding to segmental dynamics. Such scaling is similar to the result of the Zimm model although those clusters are neither chain-like nor in solution. Clusters that are larger than this critical diameter and formed by the association of giant molecules exhibit an elastic plateau due to caging of individual giant molecules. Herein, we hypothesize that clusters of such a large size cannot move as a whole, even above the glass transition temperature of the sample. They thus are “cooperative glass-like”. A structural cluster of giant molecules could be abstracted as a dynamical cluster consisting of unlinked but cooperatively mobile beads. As derived in the random first-order transition theory, the cluster loses its mobility and reaches the glassy state when the diameter of the cluster is 6 times larger than the bead diameter. In our cases, we estimate that the critical diameter for these clusters is also approximately 6 times the bead diameter based on the glassy shear modulus of giant molecules. Thus, shape-persistent giant molecules may serve as a bridge between polymers and colloids and a platform to mimic cooperative rearrangements.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC)

OSTI ID:: 1406629

Journal Information:: Macromolecules, Vol. 50, Issue 17; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: ENGLISH

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Cited by: 31 works

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A Critical Approach to Polymer Dynamics in Supramolecular Polymers Golkaram, Milad; Loos, Katja Macromolecules, Vol. 52, Issue 24 https://doi.org/10.1021/acs.macromol.9b02085	journal	December 2019

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