Abstract
Colloidal gels are elasto-plastic materials composed of an out-of-equilibrium, self-assembled network of micron-sized (solid) particles suspended in a fluid. Recent work has shown that far-field hydrodynamic interactions do not change gel structure, only the rate at which the network forms and ages. However, during gel formation, the interplay between short-ranged attractions leading to gelation and equally short-ranged hydrodynamic lubrication interactions remains poorly understood. Here, we therefore study gelation using a range of hydrodynamic descriptions: from single-body (Brownian Dynamics), to pairwise (Rotne-Prager-Yamakawa), to (non-)lubrication-corrected many-body (Stokesian Dynamics). We confirm the current understanding informed by simulations accurate in the far-field. Yet, we find that accounting for lubrication can strongly impact structure at low colloid volume fraction. Counterintuitively, strongly dissipative lubrication interactions also accelerate the aging of a gel, irrespective of colloid volume fraction. Both elements can be explained by lubrication forces facilitating collective dynamics and therefore phase-separation. Our findings indicate that despite the computational cost, lubricated hydrodynamic modeling with many-body far-field interactions is needed to accurately capture the evolution of the gel structure.
Original language | English |
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Pages (from-to) | 7388-7398 |
Number of pages | 11 |
Journal | Soft Matter |
Volume | 19 |
Issue number | 38 |
DOIs | |
Publication status | Published - 18 Sept 2023 |
Bibliographical note
Publisher Copyright:© 2023 The Royal Society of Chemistry.
Funding
The authors acknowledge NWO for funding through OCENW.KLEIN.354. We are grateful to the late Prof. James Swan for initial discussions on the possible differences between LB and SD simulations of colloidal gels. We thank Dr Andrew Fiore and Dr Madhu Majji for their help with getting PSE up and running with HOOMD-blue, as well as Dr Gwynn J. Elfring and Dr Zhouyang Ge for sharing an accelerated variant of PSE and discussing minor bugs in the resistance tensor.
Funders | Funder number |
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Nederlandse Organisatie voor Wetenschappelijk Onderzoek | OCENW.KLEIN.354 |