Constraints on Sub-GeV Dark-Matter-Electron Scattering from the DarkSide-50 Experiment.

We present new constraints on sub-GeV dark-matter particles scattering off electrons based on 6780.0 kg d of data collected with the DarkSide-50 dual-phase argon time projection chamber. This analysis uses electroluminescence signals due to ionized electrons extracted from the liquid argon target.

Low-Mass Dark Matter Search with the DarkSide-50 Experiment.

We present the results of a search for dark matter weakly interacting massive particles (WIMPs) in the mass range below 20  GeV/c^{2} using a target of low-radioactivity argon with a 6786.0 kg d exposure. The data were obtained using the DarkSide-50 apparatus at Laboratori Nazionali del Gran Sasso.

Reverse Mössbauer effect as a possible source of "hot" molecules absorbed in crystalline solids at low temperature.

As an attempt to explain some of the many anomalies and unresolved problems which have been reported about the dynamic behavior of particles and molecules absorbed in crystalline solids, the "reverse Mössbauer effect" (RME) is proposed. RME theory posits that a particle in non-equilibrium state with respect to a crystal (colliding with the crystal or absorbed in it, but set out of thermal equilibrium by some external cause) is scattered by the whole crystal with a momentum proportional to a vector representing a reciprocal lattice point. The scattering is expected to occur with a well-defined probability and the momentum transferable to the particle is expected to follow a predictable distribution.

Partial Charges in Periodic Systems: Improving Electrostatic Potential (ESP) Fitting via Total Dipole Fluctuations and Multiframe Approaches.

Two major improvements to the state-of-the-art Repeating Electrostatic Potential Extracted Atomic (REPEAT) method, for generating accurate partial charges for molecular simulations of periodic structures, are here developed. The first, D-REPEAT, consists in the simultaneous fit of the electrostatic potential (ESP), together with the total dipole fluctuations (TDF) of the framework. The second, M-REPEAT, allows the fit of multiple ESP configurations at once.

A network of discrete events for the representation and analysis of diffusion dynamics.

We developed a coarse-grained description of the phenomenology of diffusive processes, in terms of a space of discrete events and its representation as a network. Once a proper classification of the discrete events underlying the diffusive process is carried out, their transition matrix is calculated on the basis of molecular dynamics data. This matrix can be represented as a directed, weighted network where nodes represent discrete events, and the weight of edges is given by the probability that one follows the other.

The interplay between dynamic heterogeneities and structure of bulk liquid water: A molecular dynamics simulation study.

In order to study the interplay between dynamical heterogeneities and structural properties of bulk liquid water in the temperature range 130-350 K, thus including the supercooled regime, we use the explicit trend of the distribution functions of some molecular properties, namely, the rotational relaxation constants, the atomic mean-square displacements, the relaxation of the cross correlation functions between the linear and squared displacements of H and O atoms of each molecule, the tetrahedral order parameter q and, finally, the number of nearest neighbors (NNs) and of hydrogen bonds (HBs) per molecule. Two different potentials are considered: TIP4P-Ew and a model developed in this laboratory for the study of nanoconfined water. The results are similar for the dynamical properties, but are markedly different for the structural characteristics.

Combining off-lattice Monte Carlo and cellular automata for the simulation of hard-sphere systems.

In the present work we show how the update rule of a diffusive cellular automaton with mutual exclusion can be exploited in off-lattice Monte Carlo simulations of hard spheres to obtain a synchronous Monte Carlo sampling that satisfies the detailed balance principle.

Thermodynamics of the one-dimensional parallel Kawasaki model: exact solution and mean-field approximations.

The adsorption isotherm for the recently proposed parallel Kawasaki (PK) lattice-gas model [Phys. Rev. E 88, 062144 (2013)] is calculated exactly in one dimension.

A coarse-grained method based on the analysis of short molecular dynamics trajectories for the simulation of non-Markovian dynamics of molecules adsorbed in microporous materials.

We developed a coarse-grained model suitable for the study of adsorbed molecules in microporous materials. A partition of the space available to the motion of adsorbed molecules was carried out, which allows to formulate the dynamics in terms of jumps between discrete regions. The probabilities of observing given pairs of successive jumps were calculated from Molecular Dynamics (MD) simulations, performed on small systems, and used to drive the motion of molecules in a lattice-gas model.

Distributions of single-molecule properties as tools for the study of dynamical heterogeneities in nanoconfined water.

The explicit trend of the distribution functions of single-molecule rotational relaxation constants and atomic mean-square displacement are used to study the dynamical heterogeneities in nanoconfined water. The trend of the single-molecule properties distributions is related to the dynamic heterogeneities, and to the dynamic crossovers found in water clusters of different shapes and sizes and confined in a variety of zeolites. This was true in all the cases that were considered, in spite of the various shapes and sizes of the clusters.

Conciliating synchronicity with spatial discretization, exclusion, interactions, and detailed balance.

The construction of a discrete stochastic system of interacting particles that evolves through a fully synchronous evolution rule while satisfying detailed balance is a highly demanding task. As a consequence, the presence of nontrivial interaction fields can make synchronicity and thermodynamic equilibrium look as two conflicting counterparts. We show that, with the proper prescriptions, the process of migration of particles in a lattice of mutually exclusive nodes can be simulated with a fully synchronous algorithm, which we call parallel Kawasaki dynamics (PKD), that incorporates site exclusion, local interactions, and detailed balance without the need of system partitioning schemes.

Synchronous equilibrium model for the diffusion of mutually exclusive particles in a heterogeneous lattice of adsorption sites.

Through straight synchronization and proper manipulation of a sequential Monte Carlo glass-forming rule introduced by Fröbose and Jäckle [J. Stat. Phys.

Chemical potential evaluation in NVT lattice-gas simulations.

The discrete nature of the partition function of a lattice-gas system can be exploited to build an efficient strategy for the evaluation of the chemical potential of a periodic lattice-gas with arbitrarily ranged interactions during a simulation in the canonical ensemble, with the need of no additional sampling as it were required instead by the Widom insertion/deletion approach. The present method is based on the main concepts of the small system grand ensemble [for details, see G. Soto-Campos, D.

Computer simulations of dynamic crossover phenomena in nanoconfined water.

In order to study dynamic crossover phenomena in nanoconfined water we performed a series of molecular dynamics (MD) computer simulations of water clusters adsorbed in zeolites, which are microporous crystalline aluminosilicates containing channels and cavities of nanometric dimensions. We used a sophisticated empirical potential for water, including the full flexibility of the molecule and the correct response to the electric field generated by the cations and by the charged atoms of the aluminosilicate framework. In addition, the full flexibility of the aluminosilicate framework was included in the calculations.

A parallelizable block cellular automaton for the study of diffusion of binary mixtures containing CO2 in microporous materials.

We applied a method based on a block cellular automaton (BCA) algorithm to the study of diffusion of various binary mixtures adsorbed in a model microporous material, such as zeolite ZK4. Our aim was to test the capability of our model to cope with systems in which more than one species is present, using a set of parameters based on heuristic considerations from the molecular dynamics (MD) results present in the literature. A rigorous methodology for the assignment of suitable adsorption energies and diffusion activation barriers for our BCA has not been developed yet, nonetheless the results were quite interesting at this stage and we obtained a good qualitative agreement with MD data in the literature.

Speeding up simulation of diffusion in zeolites by a parallel synchronous kinetic Monte Carlo algorithm.

Understanding the behaviors of molecules in tight confinement is a challenging task. Standard simulation tools like kinetic Monte Carlo have proven to be very effective in the study of adsorption and diffusion phenomena in microporous materials, but they turn out to be very inefficient when simulation time and length scales are extended. In this paper we have explored the possibility of application of a discrete version of the synchronous parallel kinetic Monte Carlo algorithm introduced by Martínez et al.

Estimation of Partial Charges in Small Zeolite Imidazolate Frameworks from Density Functional Theory Calculations.

Zeolitic Imidazolate Frameworks (ZIFs) are the new frontier in the field of metal-organic materials. They incorporate the confining properties of the more traditional aluminosilicate zeolites together with the catalytic activity provided by transition metal ions and organic links. Computation of atomic point charges for these hybrid materials is important in the field of molecular simulations for substantial prediction of experimental results.

A molecular dynamics study and molecular level explanation of pressure dependence of ionic conductivity of potassium chloride in water.

Experimental ionic conductivity of different alkali ions in water shows markedly different dependences on pressure. Existing theories such as that of Hubbard-Onsager are unable to explain these dependences on pressure of the ionic conductivity for all ions. We report molecular dynamics investigation of potassium chloride solution at low dilution in water at several pressures between 1 bar and 2 kbar.

The central cell model: a mesoscopic hopping model for the study of the displacement autocorrelation function.

On the mesoscale, the molecular motion in a microporous material can be represented as a sequence of hops between different pore locations and from one pore to the other. On the same scale, the memory effects in the motion of a tagged particle are embedded in the displacement autocorrelation function (DACF), the discrete counterpart of the velocity autocorrelation function (VACF). In this paper, a mesoscopic hopping model, based on a lattice-gas automata dynamics, is presented for the coarse-grained modeling of the DACF in a microporous material under conditions of thermodynamic equilibrium.

The behaviour of water confined in zeolites: molecular dynamics simulations versus experiment.

In order to study the behaviour of water adsorbed in zeolites, which are microporous crystalline aluminosilicates, whose channels and cavities of nanometric dimensions can host many different molecules, we developed a sophisticated empirical potential for water, including the full flexibility of the molecule and the correct response to the electric field generated by the cations and by the charged atoms of the aluminosilicate framework. The reproduction of experimental data by our potential model is similar or even better than that obtained from the first principles methods. The results of molecular dynamics simulations of water confined in a variety of zeolites (worm-like clusters in silicalite, spherical nanoclusters in zeolite A and ice-like nanotubes in AlPO(4)-5 and SSZ-24) at different temperatures and coverage (loading) are discussed in connection with the experimental data, whose overall good reproduction encourages the attempt of an atomic-scale description of structural and dynamical phenomena occurring in confined water, in particular in the supercooled regime.

From thermodynamic cell models to partitioning cellular automata for diffusion in zeolites. II. Static and dynamic properties.

In this second paper we exploit our thermodynamic partitioning cellular automaton (PCA) developed in Paper I [Pazzona et al., J. Chem.

From thermodynamic cell models to partitioning cellular automata for diffusion in zeolites. I. Structure of the algorithm.

In the study of adsorption of simple adsorbates in microporous materials like zeolites, thermodynamic models of small grand-canonical cells with very local interactions [e.g., see K.

Effective interactions in multisite cells for adsorption in microporous materials.

Local, discrete models of self-interacting multisite adsorption cells have been shown to be able to provide a coarse-grained representation of equilibrium properties of small molecules adsorbed in nanoporous materials at the mesoscopic scale. In the present work we show how the essential statistical properties of a host cell of structured sites with multiple adsorption energies and particle-particle interactions (that is the partition function, the average energy, and the average number of guests close to the windows connecting the cell to its surroundings) can be reproduced by a less-structured cell with two occupancy-dependent adsorption energy levels.

Dynamical properties of confined water nanoclusters: Simulation study of hydrated zeolite NaA: structural and vibrational properties.

Water nanoclusters confined to zeolitic cavities have been extensively investigated by various experimental techniques. We report a series of molecular dynamics simulations at different temperatures and for water nanoclusters of different sizes in order to attempt an atomistic interpretation of the properties of these systems. The cavities of zeolite NaA are spherical in shape and about 1 nm in diameter and can host nanoclusters of water containing nearly up to 24 water molecules.

Introducing a cellular automaton as an empirical model to study static and dynamic properties of molecules adsorbed in zeolites.

A new lattice gas cellular automaton (LGCA) simulation approach to study static and dynamic properties of molecules adsorbed in zeolites is proposed. The motivation for the present work arises from the ongoing effort to develop efficient numerical tools where conventional approaches like molecular dynamics and Monte Carlo have been revealed as inefficient for a real extension of length and time scales in such inhomogeneous systems. Our LGCA is constituted by a constant number of interacting identical particles, distributed among a fixed number of identical cells arranged in a three-dimensional cubic network and performing a synchronous random walk at constant temperature.