A new Monte Carlo method for getting the density of states of atomic cluster systems

J.-M. Soudan (1) , M. Basire (1) , J.-M. Mestdagh (1) , C. Angelié (1)

1 LFP - URA 2453 - Laboratoire Francis PERRIN

A novel Monte Carlo flat histogram algorithm is proposed to get the classical density of states in terms of the potential energy, g(Ep), for systems with continuous variables such as atomic clusters. It aims at avoiding the long iterative process of the Wang-Landau method and controlling carefully the convergence, but keeping the ability to overcome energy barriers. Our algorithm is based on a preliminary mapping in a series of points (called a σ-mapping), obtained by a two-parameter local probing of g(Ep), and it converges in only two subsequent reweighting iterations on large intervals. The method is illustrated on the model system of a 432 atom cluster bound by a Rydberg type potential. Convergence properties are first examined in detail, particularly in the phase transition zone. We get g(Ep) varying by a factor 103700 over the energy range [0.01 < Ep < 6000 eV], covered by only eight overlapping intervals. Canonical quantities are derived, such as the internal energy U(T) and the heat capacity CV(T). This reveals the solid to liquid phase transition, lying in our conditions at the triple point. This phase transition is further studied by computing a Lindemann-Berry index, the atomic cluster density n(r), and the pressure, demonstrating the progressive surface melting at this triple point. Some limited results are also given for 1224 and 4044 atom clusters

Mots clés: atomic clusters; critical points; electronic density of states; Landau levels; melting; Monte Carlo methods; potential energy surfaces; Rydberg states; specific heat

Domaines: Chimie théorique et/ou physique

J.-M. Soudan, M. Basire, J.-M. Mestdagh, C. Angelié. A new Monte Carlo method for getting the density of states of atomic cluster systems. Journal of Chemical Physics, 2011, 135 (14), pp.144109. ⟨10.1063/1.3647333⟩. ⟨hal-00655984⟩