Viscoplasticity and large-scale chain relaxation in glassy-polymeric strain hardening

A simple theory for glassy polymeric mechanical response which accounts for large scale chain relaxation is presented. It captures the crossover from perfect-plastic response to strong strain hardening as the degree of polymerization $N$ increases, without invoking entanglements. By relating hardening to interactions on the scale of monomers and chain segments, we correctly predict its magnitude. Strain activated relaxation arising from the need to maintain constant chain contour length reduces the $N$ dependence of the characteristic relaxation time by a factor $\sim \dot\epsilon N$ during active deformation at strain rate $\dot\epsilon$. This prediction is consistent with results from recent experiments and simulations, and we suggest how it may be further tested experimentally.Comment: The theoretical treatment of the mechanical response has been significantly revised, and the arguments for coherent relaxation during active deformation made more transparen

Static and sliding contact of rough surfaces: effect of asperity-scale properties and long-range elastic interactions

Friction in static and sliding contact of rough surfaces is important in numerous physical phenomena. We seek to understand macroscopically observed static and sliding contact behavior as the collective response of a large number of microscopic asperities. We develop an efficient numerical framework that can be used to investigate how the macroscopic response of multiple frictional contacts depends on long-range elastic interactions, different constitutive assumptions about the deforming contacts and their local shear resistance, and surface roughness. We approximate the contact between two rough surfaces as that between a regular array of discrete deformable elements attached to a elastic block and a rigid rough surface. The deformable elements are viscoelastic or elasto/viscoplastic with a range of relaxation times, and the elastic interaction between contacts is long-range. We find that the model reproduces main macroscopic features of evolution of contact and friction for a range of constitutive models of the elements, suggesting that macroscopic frictional response is robust with respect to the microscopic behavior. Viscoelasticity/viscoplasticity contributes to the increase of friction with contact time and leads to a subtle history dependence. Interestingly, long-range elastic interactions only change the results quantitatively compared to the meanfield response. We find that sustained increase in the static friction coefficient during long hold times suggests viscoelastic response of the underlying material with multiple relaxation time scales. We also find that the experimentally observed proportionality of the direct effect in velocity jump experiments to the logarithm of the velocity jump points to a complex material-dependent shear resistance at the microscale.Comment: 33 pages, 17 figure

An Eulerian projection method for quasi-static elastoplasticity

A well-established numerical approach to solve the Navier--Stokes equations for incompressible fluids is Chorin's projection method, whereby the fluid velocity is explicitly updated, and then an elliptic problem for the pressure is solved, which is used to orthogonally project the velocity field to maintain the incompressibility constraint. In this paper, we develop a mathematical correspondence between Newtonian fluids in the incompressible limit and hypo-elastoplastic solids in the slow, quasi-static limit. Using this correspondence, we formulate a new fixed-grid, Eulerian numerical method for simulating quasi-static hypo-elastoplastic solids, whereby the stress is explicitly updated, and then an elliptic problem for the velocity is solved, which is used to orthogonally project the stress to maintain the quasi-staticity constraint. We develop a finite-difference implementation of the method and apply it to an elasto-viscoplastic model of a bulk metallic glass based on the shear transformation zone theory. We show that in a two-dimensional plane strain simple shear simulation, the method is in quantitative agreement with an explicit method. Like the fluid projection method, it is efficient and numerically robust, making it practical for a wide variety of applications. We also demonstrate that the method can be extended to simulate objects with evolving boundaries. We highlight a number of correspondences between incompressible fluid mechanics and quasi-static elastoplasticity, creating possibilities for translating other numerical methods between the two classes of physical problems.Comment: 49 pages, 20 figure

Dynamics of Viscoplastic Deformation in Amorphous Solids

We propose a dynamical theory of low-temperature shear deformation in amorphous solids. Our analysis is based on molecular-dynamics simulations of a two-dimensional, two-component noncrystalline system. These numerical simulations reveal behavior typical of metallic glasses and other viscoplastic materials, specifically, reversible elastic deformation at small applied stresses, irreversible plastic deformation at larger stresses, a stress threshold above which unbounded plastic flow occurs, and a strong dependence of the state of the system on the history of past deformations. Microscopic observations suggest that a dynamically complete description of the macroscopic state of this deforming body requires specifying, in addition to stress and strain, certain average features of a population of two-state shear transformation zones. Our introduction of these new state variables into the constitutive equations for this system is an extension of earlier models of creep in metallic glasses. In the treatment presented here, we specialize to temperatures far below the glass transition, and postulate that irreversible motions are governed by local entropic fluctuations in the volumes of the transformation zones. In most respects, our theory is in good quantitative agreement with the rich variety of phenomena seen in the simulations.Comment: 16 pages, 9 figure

Wall Adhesion and Constitutive Modelling of Strong Colloidal Gels

Wall adhesion effects during batch sedimentation of strongly flocculated colloidal gels are commonly assumed to be negligible. In this study in-situ measurements of colloidal gel rheology and solids volume fraction distribution suggest the contrary, where significant wall adhesion effects are observed in a 110mm diameter settling column. We develop and validate a mathematical model for the equilibrium stress state in the presence of wall adhesion under both viscoplastic and viscoelastic constitutive models. These formulations highlight fundamental issues regarding the constitutive modeling of colloidal gels, specifically the relative utility and validity of viscoplastic and viscoelastic rheological models under arbitrary tensorial loadings. The developed model is validated against experimental data, which points toward a novel method to estimate the shear and compressive yield strength of strongly flocculated colloidal gels from a series of equilibrium solids volume fraction profiles over various column widths.Comment: 37 pages, 12 figures, submitted to Journal of Rheolog

The nonlinear time-dependent response of isotactic polypropylene

Tensile creep tests, tensile relaxation tests and a tensile test with a constant rate of strain are performed on injection-molded isotactic polypropylene at room temperature in the vicinity of the yield point. A constitutive model is derived for the time-dependent behavior of semi-crystalline polymers. A polymer is treated as an equivalent network of chains bridged by permanent junctions. The network is modelled as an ensemble of passive meso-regions (with affine nodes) and active meso-domains (where junctions slip with respect to their positions in the bulk medium with various rates). The distribution of activation energies for sliding in active meso-regions is described by a random energy model. Adjustable parameters in the stress--strain relations are found by fitting experimental data. It is demonstrated that the concentration of active meso-domains monotonically grows with strain, whereas the average potential energy for sliding of junctions and the standard deviation of activation energies suffer substantial drops at the yield point. With reference to the concept of dual population of crystalline lamellae, these changes in material parameters are attributed to transition from breakage of subsidiary (thin) lamellae in the sub-yield region to fragmentation of primary (thick) lamellae in the post-yield region of deformation.Comment: 29 pages, 12 figure