An official website of the United States government
We probe the microstructural yielding dynamics of a concentrated colloidal system by performing creep/recovery tests with simultaneous collection of coherent scattering data via X-ray Photon Correlation Spectroscopy (XPCS). This combination of rheology and scattering allows for time-resolved observations of the microstructural dynamics as yielding occurs, which can be linked back to the applied rheological deformation to form structure–property relations. Under sufficiently small applied creep stresses, examination of the correlation in the flow direction reveals that the scattering response recorrelates with its predeformed state, indicating nearly complete microstructural recovery, and the dynamics of the system under these conditions slows considerably. Conversely, larger creep stresses increase the speed of the dynamics under both applied creep and recovery. The data show a strong connection between the microstructural dynamics and the acquisition of unrecoverable strain. By comparing this relationship to that predicted from homogeneous, affine shearing, we find that the yielding transition in concentrated colloidal systems is highly heterogeneous on the microstructural level.
more »
« less
This content will become publicly available on January 22, 2026
Linking structural and rheological memory in disordered soft materials
Linking the macroscopic flow properties and nanoscopic structure is a fundamental challenge to understanding, predicting, and designing disordered soft materials. Under small stresses, these materials are soft solids, while larger loads can lead to yielding and the acquisition of plastic strain, which adds complexity to the task. In this work, we connect the transient structure and rheological memory of a colloidal gel under cyclic shearing across a range of amplitudes via a generalized memory function using rheo-X-ray photon correlation spectroscopy (rheo-XPCS). Our rheo-XPCS data show that the nanometer scale aggregate-level structure recorrelates whenever the change in recoverable strain over some interval is zero. The macroscopic recoverable strain is therefore a measure of the nano-scale structural memory. We further show that yielding in disordered colloidal materials is strongly heterogeneous and that memories of prior deformation can exist even after the material has been subjected to flow.
more »
« less
- PAR ID:
- 10600530
- Publisher / Repository:
- Soft Matter
- Date Published:
- Journal Name:
- Soft Matter
- Volume:
- 21
- Issue:
- 4
- ISSN:
- 1744-683X
- Page Range / eLocation ID:
- 750 to 759
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
When stressed sufficiently, solid materials yield and deform plastically via reorganization of microscopic constituents. Indeed, it is possible to alter the microstructure of materials by judicious application of stress, an empirical process utilized in practice to enhance the mechanical properties of metals. Understanding the interdependence of plastic flow and microscopic structure in these nonequilibrium states, however, remains a major challenge. Here, we experimentally investigate this relationship, between the relaxation dynamics and microscopic structure of disordered colloidal solids during plastic deformation. We apply oscillatory shear to solid colloidal monolayers and study their particle trajectories as a function of shear rate in the plastic regime. Under these circumstances, the strain rate, the relaxation rate associated with plastic flow, and the sample microscopic structure oscillate together, but with different phases. Interestingly, the experiments reveal that the relaxation rate associated with plastic flow at time t is correlated with the strain rate and sample microscopic structure measured at earlier and later times, respectively. The relaxation rate, in this nonstationary condition, exhibits power-law, shear-thinning behavior and scales exponentially with sample excess entropy. Thus, measurement of sample static structure (excess entropy) provides insight about both strain rate and constituent rearrangement dynamics in the sample at earlier times.more » « less
-
Many soft materials yield under mechanical loading, but how this transition from solid-like behavior to liquid-like behavior occurs can vary significantly. Understanding the physics of yielding is of great interest for the behavior of biological, environmental, and industrial materials, including those used as inks in additive manufacturing and muds and soils. For some materials, the yielding transition is gradual, while others yield abruptly. We refer to these behaviors as being ductile and brittle. The key rheological signatures of brittle yielding include a stress overshoot in steady-shear-startup tests and a steep increase in the loss modulus during oscillatory amplitude sweeps. In this work, we show how this spectrum of yielding behaviors may be accounted for in a continuum model for yield stress materials by introducing a parameter we call the brittility factor. Physically, an increased brittility decreases the contribution of recoverable deformation to plastic deformation, which impacts the rate at which yielding occurs. The model predictions are successfully compared to results of different rheological protocols from a number of real yield stress fluids with different microstructures, indicating the general applicability of the phenomenon of brittility. Our study shows that the brittility of soft materials plays a critical role in determining the rate of the yielding transition and provides a simple tool for understanding its effects under various loading conditions.more » « less
-
Materials that exhibit yielding behavior are used in many applications, from spreadable foods and cosmetics to direct write three-dimensional printing inks and filled rubbers. Their key design feature is the ability to transition behaviorally from solid to fluid under sufficient load or deformation. Despite its widespread applications, little is known about the dynamics of yielding in real processes, as the nonequilibrium nature of the transition impedes understanding. We demonstrate an iteratively punctuated rheological protocol that combines strain-controlled oscillatory shear with stress-controlled recovery tests. This technique provides an experimental decomposition of recoverable and unrecoverable strains, allowing for solid-like and fluid-like contributions to a yield stress material’s behavior to be separated in a time-resolved manner. Using this protocol, we investigate the overshoot in loss modulus seen in materials that yield. We show that this phenomenon is caused by the transition from primarily solid-like, viscoelastic dissipation in the linear regime to primarily fluid-like, plastic flow at larger amplitudes. We compare and contrast this with a viscoelastic liquid with no yielding behavior, where the contribution to energy dissipation from viscous flow dominates over the entire range of amplitudes tested.more » « less
-
We report the effect of particle surface roughness on creep deformation and subsequent strain recovery in dense colloidal suspensions. The suspensions are composed of hard-spherelike poly(methyl methacrylate) smooth (S) and rough (R) colloids with particle volume fractions ϕS = 0.64 ± 0.01 and ϕR = 0.56 ± 0.01, corresponding to a distance of 3.0% and 3.4% based on their jamming volume fractions (ϕJS=0.66±0.01, ϕJR=0.58±0.01). The suspensions are subject to a range of shear stresses (0.01–0.07 Pa) above and below the yield stress values of the two suspensions (σyS=0.035Pa, σyR=0.02Pa). During creep, suspensions of rough colloids exhibit four to five times higher strain deformation compared to smooth colloids, irrespective of the applied stress. The interlocking of surface asperities in rough colloids is likely to generate a heterogeneous microstructure, favoring dynamic particle activity and percolation of strain heterogeneities, therefore resulting in higher magnitude of strain deformation and an earlier onset of steady flow. Strain recovery after the cessation of stress reveals a nonmonotonic recoverable strain for rough colloids, where the peak recoverable strain is observed near the yield stress, followed by a steep decline with increasing stress. This type of response suggests that frictional constraints between geometrically frustrated interlocking contacts can serve as particle bonds capable of higher elastic recovery but only near the yield stress. Understanding how particle roughness affects macroscopic creep and recovery is useful in designing yield stress fluids for additive manufacturing and product formulations.more » « less
