MolMod – an open access database of force fields for molecular simulations of fluids

The MolMod database is presented, which is openly accessible at http://molmod.boltzmann-zuse.de and contains intermolecular force fields for over 150 pure fluids at present. It was developed and is maintained by the Boltzmann-Zuse Society for Computational Molecular Engineering (BZS). The set of molecular models in the MolMod database provides a coherent framework for molecular simulations of fluids. The molecular models in the MolMod database consist of Lennard-Jones interaction sites, point charges, and point dipoles and quadrupoles, which can be equivalently represented by multiple point charges. The force fields can be exported as input files for the simulation programmes ms2 and ls1 mardyn, GROMACS, and LAMMPS. To characterise the semantics associated with the numerical database content, a force field nomenclature is introduced that can also be used in other contexts in materials modelling at the atomistic and mesoscopic levels. The models of the pure substances that are included in the database were generally optimised such as to yield good representations of experimental data of the vapour–liquid equilibrium with a focus on the vapour pressure and the saturated liquid density. In many cases, the models also yield good predictions of caloric, transport, and interfacial properties of the pure fluids. For all models, references to the original works in which they were developed are provided. The models can be used straightforwardly for predictions of properties of fluid mixtures using established combination rules. Input errors are a major source of errors in simulations. The MolMod database contributes to reducing such errors.BMBF, 01IH16008E, Verbundprojekt: TaLPas - Task-basierte Lastverteilung und Auto-Tuning in der PartikelsimulationEC/H2020/694807/EU/Enrichment of Components at Interfaces and Mass Transfer in Fluid Separation Technologies/ENRICOEC/H2020/760907/EU/Virtual Materials Market Place (VIMMP)/VIMM

Molecular thermodynamics of adsorption using discrete-potential systems

A molecular thermodynamics approach has been developed in order to describe the adsorption of fluids onto solid surfaces based on the use of discrete-potential fluid models. Using perturbation theories for fluids such as the Statistical Associating Fluid Theory (SAFT) and the Discrete Potential Theory (DPT), in combination with molecular simulation, we have formulated a two-dimensional approach to describe systems of interest for the oil industry, such as adsorption isotherms of carbon dioxide and asphaltenes

Fast, Scalable, and Interactive Software for Landau-de Gennes Numerical Modeling of Nematic Topological Defects

Numerical modeling of nematic liquid crystals using the tensorial Landau-de Gennes (LdG) theory provides detailed insights into the structure and energetics of the enormous variety of possible topological defect configurations that may arise when the liquid crystal is in contact with colloidal inclusions or structured boundaries. However, these methods can be computationally expensive, making it challenging to predict (meta)stable configurations involving several colloidal particles, and they are often restricted to system sizes well below the experimental scale. Here we present an open-source software package that exploits the embarrassingly parallel structure of the lattice discretization of the LdG approach. Our implementation, combining CUDA/C++ and OpenMPI, allows users to accelerate simulations using both CPU and GPU resources in either single- or multiple-core configurations. We make use of an efficient minimization algorithm, the Fast Inertial Relaxation Engine (FIRE) method, that is well-suited to large-scale parallelization, requiring little additional memory or computational cost while offering performance competitive with other commonly used methods. In multi-core operation we are able to scale simulations up to supra-micron length scales of experimental relevance, and in single-core operation the simulation package includes a user-friendly GUI environment for rapid prototyping of interfacial features and the multifarious defect states they can promote. To demonstrate this software package, we examine in detail the competition between curvilinear disclinations and point-like hedgehog defects as size scale, material properties, and geometric features are varied. We also study the effects of an interface patterned with an array of topological point-defects.Comment: 16 pages, 6 figures, 1 youtube link. The full catastroph

Coarse-grained models for fluids and their mixtures: Comparison of Monte Carlo studies of their phase behavior with perturbation theory and experiment

The prediction of the equation of state and the phase behavior of simple fluids (noble gases, carbon dioxide, benzene, methane, short alkane chains) and their mixtures by Monte Carlo computer simulation and analytic approximations based on thermodynamic perturbation theory is discussed. Molecules are described by coarse grained (CG) models, where either the whole molecule (carbon dioxide, benzene, methane) or a group of a few successive CH_2 groups (in the case of alkanes) are lumped into an effective point particle. Interactions among these point particles are fitted by Lennard-Jones (LJ) potentials such that the vapor-liquid critical point of the fluid is reproduced in agreement with experiment; in the case of quadrupolar molecules a quadrupole-quadrupole interaction is included. These models are shown to provide a satisfactory description of the liquid-vapour phase diagram of these pure fluids. Investigations of mixtures, using the Lorentz-Berthelot (LB) combining rule, also produce satisfactory results if compared with experiment, while in some previous attempts (in which polar solvents were modelled without explicitly taking into account quadrupolar interaction), strong violations of the LB rules were required. For this reason, the present investigation is a step towards predictive modelling of polar mixtures at low computational cost. These very simple coarse-grained models of small molecules developed here should be useful e.g. for simulations of polymer solutions with such molecules as solvent.Comment: J. Chem. Phys., accepte

Modeling the mechanics of amorphous solids at different length and time scales

We review the recent literature on the simulation of the structure and deformation of amorphous glasses, including oxide and metallic glasses. We consider simulations at different length and time scales. At the nanometer scale, we review studies based on atomistic simulations, with a particular emphasis on the role of the potential energy landscape and of the temperature. At the micrometer scale, we present the different mesoscopic models of amorphous plasticity and show the relation between shear banding and the type of disorder and correlations (e.g. elastic) included in the models. At the macroscopic range, we review the different constitutive laws used in finite element simulations. We end the review by a critical discussion on the opportunities and challenges offered by multiscale modeling and transfer of information between scales to study amorphous plasticity.Comment: 58 pages, 14 figure

Phase-field-crystal models for condensed matter dynamics on atomic length and diffusive time scales: an overview

Here, we review the basic concepts and applications of the phase-field-crystal (PFC) method, which is one of the latest simulation methodologies in materials science for problems, where atomic- and microscales are tightly coupled. The PFC method operates on atomic length and diffusive time scales, and thus constitutes a computationally efficient alternative to molecular simulation methods. Its intense development in materials science started fairly recently following the work by Elder et al. [Phys. Rev. Lett. 88 (2002), p. 245701]. Since these initial studies, dynamical density functional theory and thermodynamic concepts have been linked to the PFC approach to serve as further theoretical fundaments for the latter. In this review, we summarize these methodological development steps as well as the most important applications of the PFC method with a special focus on the interaction of development steps taken in hard and soft matter physics, respectively. Doing so, we hope to present today's state of the art in PFC modelling as well as the potential, which might still arise from this method in physics and materials science in the nearby future.Comment: 95 pages, 48 figure