Charge localization in complex oxides: Classical and quantum mechanical concepts
文献情報
In this contribution, we present a brief overview of the classical and quantum mechanical theory of charge localization in solids with application to the nonstoichiometric oxides SrFeO3−x and WO3−x. The cubic high-temperature phase of SrFeO3−x has been studied applying a Monte Carlo procedure with flexible classical charges. Oxygen vacancies exhibit a linear Fe(III)–vacancy–Fe(III) arrangement, a defect that can be described as a quadrupolaron considering its lowest nonvanishing multipole moment. This defect helps to rationalize the broad range of stability of the perovskite and the absence of polaron hopping. From a quantum mechanical perspective, we apply a nonperturbative molecular orbital approach to small polaron formation and hopping in WO3−x. A tight-binding Hamiltonian is extended by a nonretarded reaction field to account for the dielectric polarizability of the solid. The model can be solved self-consistently, leading to a localized excess charge distribution. The resulting energy barrier for polaron hopping and the impact of dynamic delocalization effects are discussed.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.











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