Ab initio calculation of the magnetic Gibbs free energy of materials using magnetically constrained supercells

Abstract

We present a first-principles approach for the computation of the magnetic Gibbs free energy of materials using magnetically constrained supercell calculations. Our approach is based on an adiabatic approximation of slowly varying local moment orientations, the so-called finite-temperature disordered local moment picture. It describes magnetic phase transitions and how electronic and/or magnetostructural mechanisms generate a discontinuous (first-order) character. We demonstrate that the statistical mechanics of the local moment orientations can be described by an affordable number of supercell calculations containing noncollinear magnetic configurations. The applicability of our approach is illustrated by firstly studying the ferromagnetic state in bcc Fe. We then investigate the temperature-dependent properties of a triangular antiferromagnetic state stabilizing in two antiperovskite systems Mn${}_3$AN (A = Ga, Ni). Our calculations provide the negative volume expansion of these materials as well as the ab initio origin of the discontinuous character of the phase transitions, electronic and/or magnetostructural, in good agreement with experiment.

arXiv comment18 pages, 10 figures

References in corpus (33)

• Skyrmion Lattice in a Chiral Magnet
• Antiferromagnetic spintronics
• Advances in the Physics of Magnetic Skyrmions and Perspective for Technology
• Electrical switching of an antiferromagnet
• On-the-fly machine learning force field generation: Application to melting points
• Magnetic skyrmion artificial synapse for neuromorphic computing
• Relativistic Neel-order fields induced by electrical current in antiferromagnets
• Anharmonic free energies and phonon dispersions from the stochastic self-consistent harmonic approximation: application to platinum and palladium hydrides
• Skyrmion-electronics: Writing, deleting, reading and processing magnetic skyrmions toward spintronic applications
• Calculating linear response functions for finite temperatures on the basis of the alloy analogy model
• Spin-order dependent anomalous Hall effect and magneto-optical effect in noncollinear antiferromagnets Mn${}_{3}X$N ($X$ = Ga, Zn, Ag, and Ni)
• Fluctuating local moments, itinerant electrons and the magnetocaloric effect: the compositional hypersensitivity of FeRh
• Equation of state of paramagnetic CrN from ab initio molecular dynamics
• Anomalous phonon lifetime shortening in paramagnetic CrN caused by magneto-lattice coupling: A combined spin and ab initio molecular dynamics study
• The anomalous Hall effect in non-collinear antiferromagnetic Mn${}_3$NiN thin films
• Piezomagnetic effect as a counterpart of negative thermal expansion in magnetically frustrated Mn-based antiperovskite nitrides
• Unified theory of electron-phonon renormalization and phonon-assisted optical absorption
• Theory of magnetic ordering in the heavy rare earths: ab-initio electronic origin of pair- and four- spin interactions
• Frustrated Magnetism and Caloric Effects in Mn-antiperovskite Nitrides: $AbInitio$ Theory
• Calculating the Magnetic Anisotropy of Rare-Earth-Transition-Metal Ferrimagnets
• Rare-earth/transition-metal magnetic interactions in pristine and (Ni,Fe)-doped YCo5 and GdCo5
• Multifunctional Antiperovskites driven by Strong Magnetostructural Coupling
• Giant Anomalous Nernst Effect in Noncollinear Antiferromagnetic Mn-based Antiperovskite Nitrides
• $\alpha$-$\beta$ phase transition of zirconium predicted by on-the-fly machine-learned force field
• Multi-site exchange enhanced barocaloric response in Mn${}_3$NiN
• Prediction of the Curie temperature considering the dependence of the phonon free energy on magnetic states
• Complex magnetism of lanthanide intermetallics unravelled
• Short period magnetization texture of B20-MnGe explained by thermally fluctuating local moments
• First-order ferromagnetic transitions of lanthanide local moments in divalent compounds: An itinerant electron positive feedback mechanism and Fermi surface topological change
• Ab initio theory of the Gibbs free energy and a hierarchy of local moment correlation functions in itinerant electron systems: The magnetism of Mn${}_3$A materials class
• Longitudinal spin fluctuations in bcc and liquid Fe at high temperature and pressure calculated with a supercell approach
• Caloric effects around phase transitions in magnetic materials described by ab initio theory: The electronic glue and fluctuating local moments
• Impact of finite temperatures on the transport properties of Gd from first principles

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