A Coarse-Grained Interaction Model for Sodium Dominant Montmorillonite.

Montmorillonite is the main crystalline mineral present in bentonite. It is an absorbent, swelling material; the physical chemistry underlying its ability to absorb water and swell occurs at the nanoscale, governed by electrical double-layer interactions. In turn, absorption and swelling lead to important changes in the macroscopic transport properties of the clay. Mesoscale models can help us establish a link between these nanoscale processes and macroscale properties, notably by providing a detailed description of its pore network. Models on the scale of hundreds to thousands of nanometers are required, which cannot realistically be handled using traditional all-atom molecular dynamics simulations. This work presents a coarse-grained (CG) mesoscale model of sodium montmorillonite. In our model, montmorillonite platelets are represented by two types of particles: central nonhydrogen-bonded particles and edge hydrogen-bonding particles. The particle interactions are described by two-body potentials, which were optimized based on all-atom molecular dynamics simulations. Specifically, several potential mean force calculations involving dry and hydrated montmorillonite were performed, using the ClayFF potential to calculate interatomic forces. The CG model was validated by testing the scalability of the model, testing its ability to reproduce potentials of mean force reported elsewhere in the literature, and by comparing the calculated elastic properties of a system containing 1000 Na montmorillonite platelets to experimentally measured elastic properties of bentonite. The simulated elastic properties obtained using our mesoscale model agree with these experimental values.

Direct Observation of Defect Range and Evolution in Ion-Irradiated Single Crystalline Ni and Ni Binary Alloys.

Energetic ions have been widely used to evaluate the irradiation tolerance of structural materials for nuclear power applications and to modify material properties. It is important to understand the defect production, annihilation and migration mechanisms during and after collision cascades. In this study, single crystalline pure nickel metal and single-phase concentrated solid solution alloys of 50%Ni50%Co (NiCo) and 50%Ni50%Fe (NiFe) without apparent preexisting defect sinks were employed to study defect dynamics under ion irradiation. Both cross-sectional transmission electron microscopy characterization (TEM) and Rutherford backscattering spectrometry channeling (RBS-C) spectra show that the range of radiation-induced defect clusters far exceed the theoretically predicted depth in all materials after high-dose irradiation. Defects in nickel migrate faster than in NiCo and NiFe. Both vacancy-type stacking fault tetrahedra (SFT) and interstitial loops coexist in the same region, which is consistent with molecular dynamics simulations. Kinetic activation relaxation technique (k-ART) simulations for nickel showed that small vacancy clusters, such as di-vacancies and tri-vacancies, created by collision cascades are highly mobile, even at room temperature. The slower migration of defects in the alloy along with more localized energy dissipation of the displacement cascade may lead to enhanced radiation tolerance.

Influence of chemical disorder on energy dissipation and defect evolution in concentrated solid solution alloys.

A grand challenge in materials research is to understand complex electronic correlation and non-equilibrium atomic interactions, and how such intrinsic properties and dynamic processes affect energy transfer and defect evolution in irradiated materials. Here we report that chemical disorder, with an increasing number of principal elements and/or altered concentrations of specific elements, in single-phase concentrated solid solution alloys can lead to substantial reduction in electron mean free path and orders of magnitude decrease in electrical and thermal conductivity. The subsequently slow energy dissipation affects defect dynamics at the early stages, and consequentially may result in less deleterious defects. Suppressed damage accumulation with increasing chemical disorder from pure nickel to binary and to more complex quaternary solid solutions is observed. Understanding and controlling energy dissipation and defect dynamics by altering alloy complexity may pave the way for new design principles of radiation-tolerant structural alloys for energy applications.