The ageing behaviour of dense suspensions or pastes at rest is almost exclusively attributed to structural dynamics. Here, we identify another ageing process, contact-controlled ageing, consisting of the progressive stiffening of solid–solid contacts of an arrested colloidal suspension. By combining rheometry, confocal microscopy and particle-scale mechanical tests using laser tweezers, we demonstrate that this process governs the shear-modulus ageing of dense aqueous silica and polymer latex suspensions at moderate ionic strengths. We further show that contact-controlled ageing becomes relevant as soon as Coulombic interactions are sufficiently screened out that the formation of solid–solid contacts is not limited by activation barriers. Given that this condition only requires moderate ion concentrations, contact-controlled ageing should be generic in a wide class of materials, such as cements, soils or three-dimensional inks, thus questioning our understanding of ageing dynamics in these systems.
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Colloidal density control with Bessel–Gauss beams
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This work benefited from a French government grant managed by ANR within the framework of the National Program Investments for the Future, ANR-11-LABX-0022-01. F.B.’s stay at the University of Delaware was supported by University Paris-Est.
The authors declare no competing interests.
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Supplementary Video, Notes 1 and 2, Methods, Figs. 1–5 and References.
Supplementary Video 1
Two videos running in parallel show the contact formation and opening tests at two ionic strengths.
Source Data Fig. 1
Shear modulus versus ageing time data.
Source Data Fig. 2
Unprocessed confocal images at ageing times t = 1, 5 and 10 min.
Source Data Fig. 3
Source data. Page 1, force versus deflection data at three ageing times and pages 2–4, deduced bond rigidity for three ionic strengths and two rod sizes.
Source Data Fig. 4
Source data. Page 1, shear modulus versus bond rigidity and page 2, S versus packing fraction.
Source Data Fig. 5
Source data. Pages 1–4, bond rigidity versus time. Pages 5 and 6, shear-modulus ageing. Page 7, shear modulus versus bond rigidity.
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Bonacci, F., Chateau, X., Furst, E.M. et al. Contact and macroscopic ageing in colloidal suspensions. Nat. Mater. 19, 775–780 (2020). https://doi.org/10.1038/s41563-020-0624-9
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