Nanoscale origins of creep in calcium silicate hydrates.

The time-dependent response of structural materials dominates our aging infrastructure's life expectancy and has important resilience implications. For calcium-silicate-hydrates, the glue of cement, nanoscale mechanisms underlying time-dependent phenomena are complex and remain poorly understood. This complexity originates in part from the inherent difficulty in studying nanoscale longtime phenomena in atomistic simulations. Herein, we propose a three-staged incremental stress-marching technique to overcome such limitations. The first stage unravels a stretched exponential relaxation, which is ubiquitous in glassy systems. When fully relaxed, the material behaves viscoelastically upon further loading, which is described by the standard solid model. By progressively increasing the interlayer water, the time-dependent response of calcium-silicate-hydrates exhibits a transition from viscoelastic to logarithmic creep. These findings bridge the gap between atomistic simulations and nanomechanical experimental measurements and pave the way for the design of reduced aging construction materials and other disordered systems such as metallic and oxide glasses

Is cement a glassy material?

The nature of Calcium-Silicate-Hydrate (C-S-H), the binding phase of cement, remains a controversial question. In particular, contrary to the former crystalline model, it was recently proposed that its nanoscale structure was actually amorphous. To elucidate this issue, we analyzed the structure of a realistic simulation of C-S-H, and compared the latter to crystalline tobermorite, a natural analogue to cement, and to an artificial ideal glass. Results clearly support that C-S-H is amorphous. However, its structure shows an intermediate degree of order, retaining some characteristics of the crystal while acquiring an overall glass-like disorder. Thanks to a detailed quantification of order and disorder, we show that its amorphous state mainly arises from its hydration. © 2014 Taylor & Francis Group

Is cement a glassy material?

The nature of Calcium-Silicate-Hydrate (C-S-H), the binding phase of cement, remains a controversial question. In particular, contrary to the former crystalline model, it was recently proposed that its nanoscale structure was actually amorphous. To elucidate this issue, we analyzed the structure of a realistic simulation of C-S-H, and compared the latter to crystalline tobermorite, a natural analogue to cement, and to an artificial ideal glass. Results clearly support that C-S-H is amorphous. However, its structure shows an intermediate degree of order, retaining some characteristics of the crystal while acquiring an overall glass-like disorder. Thanks to a detailed quantification of order and disorder, we show that its amorphous state mainly arises from its hydration. © 2014 Taylor & Francis Group

Mode Coarsening or Fracture: Energy Transfer Mechanisms in Dynamic Buckling of Rods

© 2021 American Physical Society. We present results of a hybrid experimental, theoretical, and simulation-based investigation of the postbuckling behavior of thin elastic rods axially impacted by a projectile. We find a new postbuckling mechanism: mode coarsening. Much akin to inverse energy cascade phenomena in other nonlinear dynamic systems, energy is transferred during mode coarsening from higher to lower wave numbers - unless the rod breaks, abruptly dissipating in the course of fracture the rod's strain energy. We derive a model that provides a predictive means to capture mode coarsening in the form of a nondissipative, purely geometric force relaxation mechanism, and validate the model by means of molecular dynamics (MD) based structural dynamics simulations for rods of wood and pasta considering different thermodynamic ensembles. The scalability of theory and simulation for engineering applications opens new venues toward safe design of engineering structures subject to impact-induced risks of buckling, ranging from skyscrapers, to aerospace structures, to the crashworthiness of vehicles, for example

Fracture toughness of calcium-silicate-hydrate from molecular dynamics simulations

Concrete is the most widely manufactured material in the world. Its binding phase, calcium-silicate-hydrate (C-S-H), is responsible for its mechanical properties and has an atomic structure fairly similar to that of usual calcium silicate glasses, which makes it appealing to study this material with tools and theories traditionally used for non-crystalline solids. Here, following this idea, we use molecular dynamics simulations to evaluate the fracture toughness of C-S-H, inaccessible experimentally. This allows us to discuss the brittleness of the material at the atomic scale. We show that, at this scale, C-S-H breaks in a ductile way, which prevents one from using methods based on linear elastic fracture mechanics. Knowledge of the fracture properties of C-S-H at the atomic scale opens the way for an upscaling approach to the design of tougher cement paste, which would allow for the design of slender environment-friendly infrastructures, requiring less material

Topological Origin of Fracture Toughening in Complex Solids: the Viewpoint of Rigidity Theory

In order to design tougher materials, it is crucial to understand the relationship between their composition and their resistance to fracture. To this end, we investigate the fracture toughness of usual sodium silicate glasses (NS) and complex calcium--silicate--hydrates (CSH), the binding phase of cement. Their atomistic structure is described in the framework of the topological constraints theory, or rigidity theory. We report an analogous rigidity transition, driven by pressure in NS and by composition in CSH. Relying both on simulated and available experimental results, we show that optimally constrained isostatic systems show improved fracture toughness. The flexible to stressed--rigid transition is shown to be correlated to a ductile-to-brittle transition, with a local minimum of the brittleness for isostatic system. This fracture toughening arises from a reversible molecular network, allowing optimal stress relaxation and crack blunting behaviors. This opens the way to the discovery of high-performance materials, designed at the molecular scale

Combinatorial molecular optimization of cement hydrates.

Despite its ubiquitous presence in the built environment, concrete's molecular-level properties are only recently being explored using experimental and simulation studies. Increasing societal concerns about concrete's environmental footprint have provided strong motivation to develop new concrete with greater specific stiffness or strength (for structures with less material). Herein, a combinatorial approach is described to optimize properties of cement hydrates. The method entails screening a computationally generated database of atomic structures of calcium-silicate-hydrate, the binding phase of concrete, against a set of three defect attributes: calcium-to-silicon ratio as compositional index and two correlation distances describing medium-range silicon-oxygen and calcium-oxygen environments. Although structural and mechanical properties correlate well with calcium-to-silicon ratio, the cross-correlation between all three defect attributes reveals an indentation modulus-to-hardness ratio extremum, analogous to identifying optimum network connectivity in glass rheology. We also comment on implications of the present findings for a novel route to optimize the nanoscale mechanical properties of cement hydrate