title: Residual entropy of ices and clathrates from Monte Carlo simulation.
abstract: We calculated the residual entropy of ices (Ih, Ic, III, V, VI) and clathrates (I, II, H), assuming the same energy of all configurations satisfying the Bernal-Fowler ice rules. The Metropolis Monte Carlo simulations in the range of temperatures from infinity to a size-dependent threshold were followed by the thermodynamic integration. Convergence of the simulation and the finite-size effects were analyzed using the quasichemical approximation and the Debye-Hückel theory applied to the Bjerrum defects. The leading finite-size error terms, ln N/N, 1/N, and for the two-dimensional square ice model also 1/N(3/2), were used for an extrapolation to the thermodynamic limit. Finally, we discuss the influence of unequal energies of proton configurations.
authors.affiliation: Department of Physical Chemistry, Institute of Chemical Technology, 166 28 Prague 6, Czech Republic.
authors.forename: Jiří
authors.initials: J
authors.lastname: Kolafa