Stochastic model for the dynamics of interacting Brownian particles

Using the scheme of mesoscopic nonequilibrium thermodynamics, we construct the one- and two- particle Fokker-Planck equations for a system of interacting Brownian particles. By means of these equations we derive the corresponding balance equations. We obtain expressions for the heat flux and the pressure tensor which enable one to describe the kinetic and potential energy interchange of the particles with the heat bath. Through the momentum balance we analyze in particular the diffusion regime to obtain the collective diffusion coefficient in terms of the hydrodynamic and the effective forces acting on the Brownian particles.Comment: latex fil

Crystal structure of sinhalite MgAlBO4 under high pressure

This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Physical Chemistry C, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://dx.doi.org/10.1021/jp512131eWe report on high-pressure angle-dispersive X-ray diffraction data up to 27 GPa for natural MgAlBO4 sinhalite mineral and ab initio total energy calculations. The experimental bulk modulus of sinhalite is B-0 = 171(3) GPa with a first-pressure derivative of B-0' = 4.2(3). A comparison with other olivine-type compounds shows that the value for B0 is 27% larger than that of Mg2SiO4 forsterite and 29% smaller than that of Al2BeO4 chrysoberyl. These differences are interpreted, on the basis of our ab initio calculations, in terms of the relative incompressibility of Al-O bonds in AlO6 octahedra (with a calculated bulk modulus of 250(1) GPa) as compared to Mg-O bonds in MgO6 octahedra (with a calculated bulk modulus of 130(1) GPa). The spatial cation distribution in the Pbnm orthorhombic unit cell and different polyhedral compressibilities entails a strong anisotropic compression comparable to that of forsterite. The axial compressibilities are 1.06(2) x 10(-3), 2.17(2) x 10(-3), and 1.30(3) x 10(-3) GPa(-1) for a, b, and c axes, respectively. The crystal chemistry of sinhalite under compression is compared to that of other olivine-like compounds. Compressibility trends and possible high-pressure phases are discussed.This study was supported by the Spanish government MEC under Grants No: MAT2010-21270-C04-01/03/04, MAT2013-46649-C4-1/2/3-P, and CTQ2009-14596-C02-01, by the Comunidad de Madrid and European Social Fund (S2009/PPQ1551 4161893), by MALTA Consolider Ingenio 2010 project (CSD2007-00045), and by Generalitat Valenciana (GVA-ACOMP-2013-1012 and GVA-ACOMP-2014-243). Experiments were performed at MSPD beamline at ALBA Synchrotron Light Facility with the collaboration of ALBA staff A.M. and P.R-H. acknowledge computing time provided by Red Espanola de Supercomputacion (RES) and MALTA-Cluster. J.A.S. acknowledges financial support through the Juan de la Cierva fellowship. We are particularly grateful to Angel Vegas for stimulating discussions and critical reading of this manuscript.Santamaría Pérez, D.; Errandonea, D.; Gomis, O.; Sans Tresserras, JÁ.; Pereira, ALJ.; Manjón Herrera, FJ.; Popescu, C.... (2015). Crystal structure of sinhalite MgAlBO4 under high pressure. Journal of Physical Chemistry C. 119(12):6777-6784. https://doi.org/10.1021/jp512131eS677767841191

Compression of Silver Sulfide: X-ray Diffraction Measurements and Total-Energy Calculations

Angle-dispersive X-ray diffraction measurements have been performed in acanthite, Ag₂S, up to 18 GPa in order to investigate its high-pressure structural behavior. They have been complemented by ab initio electronic structure calculations. From our experimental data, we have determined that two different high-pressure phase transitions take place at 5 and 10.5 GPa. The first pressure-induced transition is from the initial anti-PbCl₂-like monoclinic structure (space group <i>P</i>2₁/<i>n</i>) to an orthorhombic Ag₂Se-type structure (space group <i>P</i>2₁2₁2₁). The compressibility of the lattice parameters and the equation of state of both phases have been determined. A second phase transition to a <i>P</i>2₁/<i>n</i> phase has been found, which is a slight modification of the low-pressure structure (Co₂Si-related structure). The initial monoclinic phase was fully recovered after decompression. Density functional and, in particular, GGA+U calculations present an overall good agreement with the experimental results in terms of the high-pressure sequence, cell parameters, and their evolution with pressure