Anisotropic and heterogeneous dynamics in an aging colloidal gel

Jain, Avni; Schulz, Florian; Lokteva, Irina; Frenzel, Lara; Grübel, G.; Lehmkühler, Felix

doi:10.1039/c9sm02230a

Cited by 24 publications

(22 citation statements)

References 67 publications

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“…Our results clearly show that the coarsening dynamics of the protein droplets at this length scale are not governed by Brownian dynamics but instead by a ballistic and partially cooperative motion of the protein droplets driven by the spinodal decomposition. Similar super diffusive ballistic types of dynamics have been observed frequently in soft matter systems, e.g., in the late stage of colloidal gelation processes [52][53][54], during spinodal decomposition of colloidal systems [27], and in the framework of MD simulations of metallic glasses [55] with strongly interconnected clusters moving together. Phenomenological models of single microcollapse events PHYSICAL REVIEW LETTERS 126, 138004 (2021)…”

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confidence: 68%

Microscopic Dynamics of Liquid-Liquid Phase Separation and Domain Coarsening in a Protein Solution Revealed by X-Ray Photon Correlation Spectroscopy

et al. 2021

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While the interplay between liquid-liquid phase separation (LLPS) and glass formation in biological systems is highly relevant for their structure formation and thus function, the exact underlying mechanisms are not well known. The kinetic arrest originates from the slowdown at the molecular level, but how this propagates to the dynamics of microscopic phase domains is not clear. Since with diffusion, viscoelasticity, and hydrodynamics, distinctly different mechanisms are at play, the dynamics needs to be monitored on the relevant time and length scales and compared to theories of phase separation. Using x-ray photon correlation spectroscopy, we determine the LLPS dynamics of a model protein solution upon low temperature quenches and find distinctly different dynamical regimes. We observe that the early stage LLPS is driven by the curvature of the free energy and speeds up upon increasing quench depth. In contrast, the late stage dynamics slows down with increasing quench depth, fingerprinting a nearby glass transition. The dynamics observed shows a ballistic type of motion, implying that viscoelasticity plays an important role during LLPS. We explore possible explanations based on the Cahn-Hilliard theory with nontrivial mobility parameters and find that these can only partially explain our findings.

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confidence: 68%

Microscopic Dynamics of Liquid-Liquid Phase Separation and Domain Coarsening in a Protein Solution Revealed by X-Ray Photon Correlation Spectroscopy

et al. 2021

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“…As introduced above, the use of higher-order correlation functions reveals non-equilibrium processes by accessing the age-dependence of the relaxation time in real-time experiments. Dynamical heterogeneities are particularly present in gels [47,104,105], elastomers [106], in glasses and close to the glass transition [29,[107][108][109][110], as well as reported recently during liquid-liquid separations in dense protein dispersions [39]. Here, we want to highlight few recent examples.…”

Section: Dynamical Heterogeneities Via Two-times Correlationsmentioning

confidence: 70%

“…Recently, thanks to the increased detector performance and coherent flux, direction-dependent structural heterogeneities could be accessed for different samples, calculated from fractions of pixels. Jain et al studied the aging of a colloidal gel after quenching it close to and below the gelation point [105]. Stress-induced microcollapses were found to couple with cooperative rearrangements on larger scales, as indicated by dynamical heterogeneities at small q.…”

Section: Dynamical Heterogeneities Via Two-times Correlationsmentioning

confidence: 99%

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From Femtoseconds to Hours—Measuring Dynamics over 18 Orders of Magnitude with Coherent X-rays

2021

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X-ray photon correlation spectroscopy (XPCS) enables the study of sample dynamics between micrometer and atomic length scales. As a coherent scattering technique, it benefits from the increased brilliance of the next-generation synchrotron radiation and Free-Electron Laser (FEL) sources. In this article, we will introduce the XPCS concepts and review the latest developments of XPCS with special attention on the extension of accessible time scales to sub-μs and the application of XPCS at FELs. Furthermore, we will discuss future opportunities of XPCS and the related technique X-ray speckle visibility spectroscopy (XSVS) at new X-ray sources. Due to its particular signal-to-noise ratio, the time scales accessible by XPCS scale with the square of the coherent flux, allowing to dramatically extend its applications. This will soon enable studies over more than 18 orders of magnitude in time by XPCS and XSVS.

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“…Area detectors allow multiple intensity-time series to be measured simultaneously, improving the equilibrium g 2 SNR by (N p ) 1/2 , while also providing concurrent measurements of the Q dependence of g 2 , thereby improving the efficiency of measurements. In the case of two-time measurements where the dynamics evolve over time (Fluerasu et al, 2005;Madsen et al, 2010;Das et al, 2019;Mokhtarzadeh et al, 2019;Hoshino et al, 2020;Jain et al, 2020), the SNR does not improve by increasing N f since the correlation is calculated between two frames, making the large N p provided by an area detector the only way to maintain the SNR of the correlation without sacrificing the time resolution indicated by t e .…”

Section: Introductionmentioning

confidence: 99%

20 µs-resolved high-throughput X-ray photon correlation spectroscopy on a 500k pixel detector enabled by data-management workflow

Zhang¹,

Đufresne²,

Nakaye³

et al. 2021

J Synchrotron Rad

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The performance of the new 52 kHz frame rate Rigaku XSPA-500k detector was characterized on beamline 8-ID-I at the Advanced Photon Source at Argonne for X-ray photon correlation spectroscopy (XPCS) applications. Due to the large data flow produced by this detector (0.2 PB of data per 24 h of continuous operation), a workflow system was deployed that uses the Advanced Photon Source data-management (DM) system and high-performance software to rapidly reduce area-detector data to multi-tau and two-time correlation functions in near real time, providing human-in-the-loop feedback to experimenters. The utility and performance of the workflow system are demonstrated via its application to a variety of small-angle XPCS measurements acquired from different detectors in different XPCS measurement modalities. The XSPA-500k detector, the software and the DM workflow system allow for the efficient acquisition and reduction of up to ∼109 area-detector data frames per day, facilitating the application of XPCS to measuring samples with weak scattering and fast dynamics.

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Anisotropic and heterogeneous dynamics in an aging colloidal gel

Abstract: We investigate the out-of-equilibrium dynamics of a colloidal gel obtained by quenching a suspension of soft polymer-coated gold nanoparticles close to and below its gelation point using X-ray Photon Correlation Spectroscopy (XPCS).

Cited by 24 publications

References 67 publications

Microscopic Dynamics of Liquid-Liquid Phase Separation and Domain Coarsening in a Protein Solution Revealed by X-Ray Photon Correlation Spectroscopy

Microscopic Dynamics of Liquid-Liquid Phase Separation and Domain Coarsening in a Protein Solution Revealed by X-Ray Photon Correlation Spectroscopy

From Femtoseconds to Hours—Measuring Dynamics over 18 Orders of Magnitude with Coherent X-rays

20 µs-resolved high-throughput X-ray photon correlation spectroscopy on a 500k pixel detector enabled by data-management workflow

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