Isotropic-to-Nematic Transition in Salt-Free Polyelectrolyte Coacervates from Coarse-Grained Simulations

Yu, Boyuan; Liang, Heyi; Rumyantsev, Artem M.; de Pablo, Juan J.

doi:10.1021/acs.macromol.2c01674

Isotropic-to-Nematic Transition in Salt-Free Polyelectrolyte Coacervates from Coarse-Grained Simulations

Journal Article · Tue Oct 18 00:00:00 EDT 2022 · Macromolecules

DOI:https://doi.org/10.1021/acs.macromol.2c01674· OSTI ID:2437749

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Univ. of Chicago, IL (United States)
Univ. of Chicago, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Recent interest in complex coacervation between oppositely charged polyelectrolytes (PEs) has been fueled by its relevance to biology in the context of membraneless organelle formation within living cells. For PEs with limited flexibility (such as double-stranded DNA), theoretical treatments and recent experiments have reported the emergence of liquid crystalline order (LCO) within the resulting coacervate phases. In this work, we study the underlying physics of this phenomenon using coarse-grained molecular dynamics simulations of symmetric semiflexible-semiflexible and asymmetric semiflexible-flexible coacervates. By comparing coacervates with the corresponding semidilute solutions of neutral polymers, we demonstrate that the presence of Coulomb interactions in coacervates facilitates orientational ordering, in agreement with theoretical predictions. Quantitative comparisons between our simulations and theory indicate that, for asymmetric nematic coacervates, the strong orientational ordering of stiff polyanions induces a weak ordering of the flexible polycations-an effect that was not anticipated by available theoretical studies. Simulations reveal that, for nematic coacervates, the preferred orientation of the PE chains at the liquid-liquid coacervate-supernatant interface is parallel, and the alignment of semiflexible PEs is homogeneous. The results presented here provide new molecular-level insights into the intracoacervate LCO and will help motivate further experimental and theoretical activities in this area.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2437749

Journal Information:: Macromolecules, Journal Name: Macromolecules Journal Issue: 21 Vol. 55; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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