Papers by Author: Bernard Legrand

Abstract: Surface segregation in transition metals can be analysed within a generalised Ising model,derived from Tight-Binding electronic structure calculations, which identifies three driving forces:the difference in surface energy and atomic volume between the two components and their tendencyto order or phase separate in the bulk. Using this ”three effects” rule, we present here general mapswhich predict the tendency of the solute metal element to segregate (or not) at the surface of a metalmatrix, for the 702 solute/matrix systems that can be formed with transition metal elements. Ourpredictions compare fairly well to the existing ab initio calculations and experimental data availableon these systems. The few exceptions, which mainly concern given matrix elements are discussed indetails.

Abstract: We compare three models of 2D precipitation kinetics that give access to different time-space scales. Kinetic Monte Carlo simulations (KMC), cluster dynamics (CD) and nucleation-growth-coalescence model (NGCM), based on a same atomic model, lead to an excellent agreement as long as the interfacial free energy is evaluated accurately and the interaction between diffusion fields is taken into account in the CD. The NGCM model noticeably improves the previous approaches of the same kind by using a constrained-equilibrium hypothesis to describe the solid solution. Moreover, in the coalescence regime, we show that CD leads to cluster distributions that are wider and more symmetric than the LSW distribution due to the probabilistic feature of the growth law of a cluster, that makes it differ from the purely deterministic NGCM approach.

Abstract: In order to build the phase diagram of Cu-Ag nanoalloys, we study a 405-atom nanoparticle by means of Monte Carlo simulations with relaxations using N-body interatomic potentials. We focus on a range of nominal concentrations for which the cluster core remains Cu-pure and the (001) facets of the outer shell exhibit two original phenomena. Within the (N,m_Ag-m_Cu,P,T) ensemble, a structural and chemical bistability is observed, which affects all the (001) facets together. For a nanoparticle assembly, this will result in a bimodal distribution of clusters, some of them having their (001) facets Cu-rich with the usual square shape, the other ones having their (001) facets Ag-rich with a diamond shape. This bistability is replaced in the (N_Ag,N_Cu,P,T) ensemble by a continuous evolution of both the structure and the concentration of the (001) facets from Cu-rich square-shaped to Ag-rich diamond-shaped facets as the number of Ag atoms increases. For a nanoparticle assembly, this will result in an unimodal distribution of the cluster population concerning the properties of the (001) facets. This comparison between pseudo grand canonical and isothermal-isobaric results shows that the distribution of a population of bimetallic nanoparticles depends strongly on the conditions under it is elaborated.