Liquid structure of bistable responsive macromolecules using mean-field density-functional theory

Abstract

Macromolecular crowding typically applies to biomolecular and polymer-based systems in which the individual particles often feature a two-state folded/unfolded or coil-to-globule transition, such as found for proteins and peptides, DNA and RNA, or supramolecular polymers. Here, we employ a mean-field density functional theory (DFT) of a model of soft and bistable responsive colloids (RCs) in which the size of the macromolecule is explicitly resolved as a degree of freedom living in a bimodal 'Landau' energy landscape (exhibiting big and small states), thus directly responding to the crowding environment. Using this RC-DFT we study the effects of self-crowding on the liquid bulk structure and thermodynamics for different energy barriers and softnesses of the bimodal energy landscape, in conditions close to the coil-to-globule transition. We find substantial crowding effects on the internal distributions, a complex polydispersity behavior, and quasi-universal compression curves for increasing (generalized) packing fractions. Moreover, we uncover distinct signatures of bimodal versus unimodal behavior in the particle compression. Finally, the analysis of the pair structure - derived from the test particle route - reveals that the microstructure of the liquid is quite inhomogeneous due to local depletion effects, tuneable by particle softness.

Article information

Article type
Paper
Submitted
21 Nov 2022
Accepted
16 Mar 2023
First published
17 Mar 2023
This article is Open Access
Creative Commons BY-NC license

Soft Matter, 2023, Accepted Manuscript

Liquid structure of bistable responsive macromolecules using mean-field density-functional theory

A. Moncho Jorda, N. Göth and J. Dzubiella, Soft Matter, 2023, Accepted Manuscript , DOI: 10.1039/D2SM01523D

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