Oxidation State Dynamics and Emerging Patterns in Magnetite

Abstract

Magnetite is an important mineral with many interesting applications related to its magnetic, electrical and thermal properties. Typically studied by electronic structure calculations, these methods are unable to capture the complex ion dynamics at relevant temperatures, time and length scales. We present a hybrid Monte Carlo/Molecular Dynamics (MC/MD) method based on iron oxidation state exchange for accurate atomistic modelling of bulk magnetite, magnetite surfaces and nanoparticles that captures the complex ionic dynamics. By comparing oxidation state patterns with those obtained from density functional theory, we confirmed the accuracy of our approach. Lattice distortions leading to the stabilisation of excess charges and a critical surface thickness at which the oxidation states transition from ordered to disordered were observed. This simple yet efficient approach paves the way for elucidating aspects of oxidation state ordering of inverse spinel structures in general and battery materials in particular.

References in corpus (14)

• Iron Oxide Surfaces
• A scalable parallel Monte Carlo algorithm for atomistic simulations of precipitation in alloys
• Subsurface Cation Vacancy Stabilization of the Magnetite (001) Surface
• Jahn-Teller stabilization of a "polar" metal oxide surface: Fe3O4(001)
• Jahn-Teller distortion driven magnetic polarons in magnetite
• Electronic Orders in the Verwey Structure of Magnetite
• Insights into lithium manganese oxide-water interfaces using machine learning potentials
• Closing the gap between theory and experiment for lithium manganese oxide spinels using a high-dimensional neural network potential
• Short-Range Correlations in Magnetite above the Verwey Temperature
• Discovery of the soft electronic modes of the trimeron order in magnetite
• Shaping Magnetite Nanoparticles from First-principles
• Trimeron-phonon coupling in magnetite
• Parametrization of the Fe-Owater cross-interaction for a more accurate Fe3O4/water interface model and its application to a spherical Fe3O4 nanoparticle of realistic size
• Oxygen-Terminated (1x1) Reconstruction of Reduced Magnetite Fe${}_3$O${}_4$(111)

Cited by in corpus (2)

• Phonon density of states of magnetite (\ce{Fe3O4}) nanoparticles via molecular dynamics simulations
• Atomistic modeling of functionalized magnetite surfaces with oxidation states