Interplay between Kinetics and Dynamics of Liquid-Liquid Phase Separation in a Protein Solution Revealed by Coherent X-ray Spectroscopy

Fuente: arXiv
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Autori principali: Ragulskaya, Anastasia, Begam, Nafisa, Girelli, Anita, Rahmann, Hendrik, Reiser, Mario, Westermeier, Fabian, Sprung, Michael, Zhang, Fajun, Gutt, Christian, Schreiber, Frank
Natura: Preprint
Pubblicazione: 2021
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author Ragulskaya, Anastasia
Begam, Nafisa
Girelli, Anita
Rahmann, Hendrik
Reiser, Mario
Westermeier, Fabian
Sprung, Michael
Zhang, Fajun
Gutt, Christian
Schreiber, Frank
author_facet Ragulskaya, Anastasia
Begam, Nafisa
Girelli, Anita
Rahmann, Hendrik
Reiser, Mario
Westermeier, Fabian
Sprung, Michael
Zhang, Fajun
Gutt, Christian
Schreiber, Frank
contents Microscopic dynamics of complex fluids in the early stage of spinodal decomposition (SD) is strongly intertwined with the kinetics of structural evolution, which makes a quantitative characterization challenging. In this work, we use x-ray photon correlation spectroscopy to study the dynamics and kinetics of a protein solution undergoing liquid-liquid phase separation (LLPS). We demonstrate that in the early stage of SD, the structural relaxation kinetics is up to 40 times slower than the dynamics and thus can be decoupled. The kinetic decay rate is inversely proportional to time in the early stage, followed by a nearly constant behavior during the coarsening stage. The microscopic dynamics can be well described by hyper-diffusive ballistic motions with a relaxation time exponentially growing with time in the early stage followed by a power-law increase with fluctuations. These experimental results are further supported by simulations based on the Cahn-Hilliard equation. The established framework is applicable to other condensed matter and biological systems undergoing phase transitions and may also inspire further theoretical work.
format Preprint
id arxiv_https___arxiv_org_abs_2104_05780
institution arXiv
publishDate 2021
record_format arxiv
spellingShingle Interplay between Kinetics and Dynamics of Liquid-Liquid Phase Separation in a Protein Solution Revealed by Coherent X-ray Spectroscopy
Ragulskaya, Anastasia
Begam, Nafisa
Girelli, Anita
Rahmann, Hendrik
Reiser, Mario
Westermeier, Fabian
Sprung, Michael
Zhang, Fajun
Gutt, Christian
Schreiber, Frank
Soft Condensed Matter
Microscopic dynamics of complex fluids in the early stage of spinodal decomposition (SD) is strongly intertwined with the kinetics of structural evolution, which makes a quantitative characterization challenging. In this work, we use x-ray photon correlation spectroscopy to study the dynamics and kinetics of a protein solution undergoing liquid-liquid phase separation (LLPS). We demonstrate that in the early stage of SD, the structural relaxation kinetics is up to 40 times slower than the dynamics and thus can be decoupled. The kinetic decay rate is inversely proportional to time in the early stage, followed by a nearly constant behavior during the coarsening stage. The microscopic dynamics can be well described by hyper-diffusive ballistic motions with a relaxation time exponentially growing with time in the early stage followed by a power-law increase with fluctuations. These experimental results are further supported by simulations based on the Cahn-Hilliard equation. The established framework is applicable to other condensed matter and biological systems undergoing phase transitions and may also inspire further theoretical work.
title Interplay between Kinetics and Dynamics of Liquid-Liquid Phase Separation in a Protein Solution Revealed by Coherent X-ray Spectroscopy
topic Soft Condensed Matter
url https://arxiv.org/abs/2104.05780