Correlation effects in magnetic materials: An ab initio investigation on electronic structure and spectroscopy

Various technical developments enlarged the potential of angle-resolved photoemission spectroscopy (ARPES) tremendously during the last two decades. In particular improved momentum and energy resolution in combination with spin-resolution as well as the use of photon energies from few eV up to several keV makes ARPES a rather unique tool to investigate the electronic properties of solids and surfaces. Obviously, this rises the need for a corresponding theoretical formalism that allows to accompany experimental ARPES studies in an adequate way. As will be demonstrated by several examples this goal could be achieved by various recent developments on the basis of density functional theory (DFT) in combination with dynamical mean field theory (DMFT) and with the one-step model of photoemission (1SM). A concrete realization of electronic structure calculations in the framework of multiple scattering theory further more provides direct access to the spectral function of the initial states via the one-electron Green function. Based on this bare spectral function matrix-element and final-state effects as well as surface related features may be calculated in addition using the one-step formalism that offers the possibility to analyse corresponding angle-resolved photoemission experiments in a quantitative sense. The impact of chemical disorder can be handled by means of the coherent potential approximation (CPA) alloy theory, in the electronic structure calculation as well as in the photoemission analyses. The same holds for the influence of electronic correlation effects. These are accounted for by means of the DMFT that removes the most serious short comings of calculations based on the standard local spin density approximation (LSDA). The self-consistent combination of this approach with the CPA allows, for example, the investigation of correlated transition metal alloys. Finally, accounting for the photon momentum and going beyond the single scatterer approximation for the final state allows to deal quantitatively with ARPES in the high-energy regime (HAXPES) that reduces the influence of the surface on the spectra and therefore probes primarily the bulk electronic structure this way.

► We compare spin-resolved ARPES data of ferromagnetic 3d transition metals to many-body LSDA + DMFT based spectroscopic calculations. ► We document LSDA + DMFT provides a detailed and reliable interpretation of the data. ► We demonstrate that local correlations are dominant in Ni, whereas non-local correlations are important in Fe and Co. ► We reproduce the 6 eV satellite structure in ferromagnetic Ni LDSDA + DMFT in combination with the one-step model of photoemission provides a more or less complete description of the electronic structure of Fe, Co and Ni.