naa a22 4500 510772412 CHVBK 20180411083218.0 cr unu---uuuuu 180411e20131101xx s 000 0 eng 10.1007/s11837-013-0764-3 doi (NATIONALLICENCE)springer-10.1007/s11837-013-0764-3 van de Walle Axel School of Engineering, Brown University, Box D, 02912, Providence, RI, USA aut Methods for First-Principles Alloy Thermodynamics [Elektronische Daten] [Axel van de Walle] Traditional first-principles calculations excel at providing formation energies at absolute zero, but obtaining thermodynamic information at nonzero temperatures requires suitable sampling of all the excited states visited in thermodynamic equilibrium, which would be computationally prohibitive via brute-force quantum mechanical calculations alone. In the context of solid-state alloys, this issue can be addressed via the coarse-graining concept and the cluster expansion formalism. This process generates simple, effective Hamiltonians that accurately reproduce quantum mechanical calculation results and that can be used to efficiently sample configurational, vibrational, and electronic excitations and enable the prediction of thermodynamic properties at nonzero temperatures. Vibrational and electronic degrees of freedom are formally eliminated from the problem by writing the system's partition function in a nested form in which the inner sums can be readily evaluated to yield an effective Hamiltonian. The remaining outermost sum corresponds to atomic configurations and can be handled via Monte Carlo sampling driven by the resulting effective Hamiltonian, thereby delivering thermodynamic properties at nonzero temperatures. This article describes these techniques and their implementation in the alloy theoretic automated toolkit, an open-source software package. The methods are illustrated by applications to various alloy systems. The Minerals, Metals & Materials Society, 2013 JOM Springer US; http://www.springer-ny.com 65/11(2013-11-01), 1523-1532 1047-4838 65:11<1523 2013 65 11837 https://doi.org/10.1007/s11837-013-0764-3 text/html Onlinezugriff via DOI 1 research-article jats NATIONALLICENCE 856 40 https://doi.org/10.1007/s11837-013-0764-3 text/html Onlinezugriff via DOI NATIONALLICENCE 100 1- van de Walle Axel School of Engineering, Brown University, Box D, 02912, Providence, RI, USA aut NATIONALLICENCE 773 0- JOM Springer US; http://www.springer-ny.com 65/11(2013-11-01), 1523-1532 1047-4838 65:11<1523 2013 65 11837 Metadata rights reserved Springer special CC-BY-NC licence nationallicence BK010053 XK010053 XK010000 NATIONALLICENCE NATIONALLICENCE NL-springer