Transfer matrix theory of polymer complex coacervation

Soft Matter ◽  
2017 ◽  
Vol 13 (39) ◽  
pp. 7001-7012 ◽  
Author(s):  
Tyler K. Lytle ◽  
Charles E. Sing

A new theoretical approach to modeling polymeric complex coacervation captures how molecular features affect charge-driven phase separation.

Soft Matter ◽  
2019 ◽  
Vol 15 (44) ◽  
pp. 9157-9158
Author(s):  
Tyler K. Lytle ◽  
Charles E. Sing

Correction for ‘Transfer matrix theory of polymer complex coacervation’ by Tyler K. Lytle et al., Soft Matter, 2017, 13, 7001–7012.


2018 ◽  
Vol 3 (1) ◽  
pp. 183-196 ◽  
Author(s):  
Tyler K. Lytle ◽  
Charles E. Sing

Theory and simulation demonstrate how molecular features can be used to design the phase behavior of polymeric complex coacervates.


Author(s):  
Fatma Pir Cakmak ◽  
Saehyun Choi ◽  
McCauley O. Meyer ◽  
Philip C. Bevilacqua ◽  
Christine D. Keating

AbstractMultivalent polyions can undergo complex coacervation, producing membraneless compartments that accumulate ribozymes and enhance catalysis, and offering a mechanism for functional prebiotic compartmentalization in the origins of life. Here, we evaluated the impact of low, prebiotically-relevant polyion multivalency in coacervate performance as functional compartments. As model polyions, we used positively and negatively charged homopeptides with one to 100 residues, and adenosine mono-, di-, and triphosphate nucleotides. Polycation/polyanion pairs were tested for coacervation, and resulting membraneless compartments were analyzed for salt resistance, ability to provide a distinct internal microenvironment (apparent local pH, RNA partitioning), and effect on RNA structure formation. We find that coacervates formed by phase separation of the relatively shorter polyions more effectively generated distinct pH microenvironments, accumulated RNA, and preserved duplexes. Hence, reduced multivalency polyions are not only viable as functional compartments for prebiotic chemistries, but they can offer advantages over higher molecular weight analogues.


2020 ◽  
Vol 11 (1) ◽  
Author(s):  
Fatma Pir Cakmak ◽  
Saehyun Choi ◽  
McCauley O. Meyer ◽  
Philip C. Bevilacqua ◽  
Christine D. Keating

AbstractMultivalent polyions can undergo complex coacervation, producing membraneless compartments that accumulate ribozymes and enhance catalysis, and offering a mechanism for functional prebiotic compartmentalization in the origins of life. Here, we evaluate the impact of lower, more prebiotically-relevant, polyion multivalency on the functional performance of coacervates as compartments. Positively and negatively charged homopeptides with 1–100 residues and adenosine mono-, di-, and triphosphate nucleotides are used as model polyions. Polycation/polyanion pairs are tested for coacervation, and resulting membraneless compartments are analyzed for salt resistance, ability to provide a distinct internal microenvironment (apparent local pH, RNA partitioning), and effect on RNA structure formation. We find that coacervates formed by phase separation of the shorter polyions more effectively generated distinct pH microenvironments, accumulated RNA, and preserved duplexes than those formed by longer polyions. Hence, coacervates formed by reduced multivalency polyions are not only viable as functional compartments for prebiotic chemistries, they can outperform higher molecular weight analogues.


2019 ◽  
Vol 10 (9) ◽  
pp. 2700-2707 ◽  
Author(s):  
Rachel A. Kapelner ◽  
Allie C. Obermeyer

Short ionic polypeptide tags were demonstrated to drive complex coacervation of globular proteins at physiological conditions while maintaining protein activity.


Soft Matter ◽  
2020 ◽  
Vol 16 (12) ◽  
pp. 2885-2914 ◽  
Author(s):  
Charles E. Sing ◽  
Sarah L. Perry

We review recent progress in the science of polymeric complex coacervation.


2021 ◽  
Author(s):  
Krishna Shrinivas ◽  
Michael P Brenner

Fluids in natural systems, like the cytoplasm of a cell, often contain thousands of molecular species that are organized into multiple coexisting phases that enable diverse and specific functions. How interactions between numerous molecular species encode for various emergent phases is not well understood. Here we leverage approaches from random matrix theory and statistical physics to describe the emergent phase behavior of fluid mixtures with many species whose interactions are drawn randomly from an underlying distribution. Through numerical simulation and stability analyses, we show that these mixtures exhibit staged phase separation kinetics and are characterized by multiple coexisting phases at equilibrium with distinct compositions. Random-matrix theory predicts the number of existing phases at equilibrium, validated by simulations with diverse component numbers and interaction parameters. Surprisingly, this model predicts an upper bound on the number of phases, derived from dynamical considerations, that is much lower than the limit from the Gibbs phase rule, which is obtained from equilibrium thermodynamic constraints. Using a biophysically motivated model of pairwise interactions between components, we design ensembles that encode either linear or non-monotonic scaling relationships between number of components and co-existing phases, which we validate through simulation and theory. Finally, inspired by parallels in biological systems, we show that including non-equilibrium turnover of components through chemical reactions can tunably modulate the number of co-existing phases at steady-state without changing overall fluid composition. Together, our study provides a model framework that describes the emergent dynamical and steady-state phase behavior of liquid-like mixtures with many interacting constituents.


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