2006/10/13 by Fei Zhou, Thomas Maxisch, Gerbrand Ceder · 244 citations
Materials Science · Physics and Astronomy · #Ab initio #Chemical physics #Condensed matter physics #Configuration entropy #Electronic structure #Ion #Ionic bonding #Lattice (music) #Machine Learning in Materials Science #Magnetic and transport properties of perovskites and related materials #Materials science #Phase (matter) #Phase diagram #Physics #Quantum mechanics #Statistical physics #Thermodynamics #Transition Metal Oxide Nanomaterials #Valence (chemistry) #cond-mat.mtrl-sci
paper · pdf · doi:10.1103/physrevlett.97.155704
published in Physical Review Letters 97(15), 155704 (American Physical Society) · 4 figures
openalex publication_date 2006/10/13 · arxiv created 2006/12/06 · arxiv updated 2015/11/17 · openalex created_date 2016/06/24 · openalex updated_date 2026/08/05
We demonstrate that configurational electronic entropy, previously neglected, in ab initio thermodynamics of materials can qualitatively modify the finite-temperature phase stability of mixed-valence oxides. While transformations from low-T ordered or immiscible states are almost always driven by configurational disorder (i.e., random occupation of lattice sites by multiple species), in FePO4-LiFePO4 the formation of a solid solution is almost entirely driven by electronic rather than ionic configurational entropy. We argue that such an electronic entropic mechanism may be relevant to most other mixed-valence systems.