Abstract
A fully relativistic theory of angle-resolved two-photon photoemission for ferromagnetic materials is derived from the general theory of pump-probe photoemission that is based on the Keldysh formalism. Two-photon photoemission spectroscopy is a widely used analytical tool to study nonequilibrium phenomena in nonmagnetic as well as in magnetic solids, as for example ultrafast demagnetization processes. Our theoretical approach aims at a quantitative description of the time-dependent spectroscopic properties of specific solid systems under consideration, and it allows for the inclusion of static correlation effects via the local spin-density and dynamical mean-field theory electronic structure approach. To this end we follow Pendry's one-step theory of the photoemission process as closely as possible and make extensive use of concepts of relativistic multiple - scattering theory within the layer-Korringa-Kohn-Rostoker method in order to guarantee angular resolution in the spectroscopic calculations. As usual the final state of the two-photon photoemission process is represented by a time-reversed low-energy electron diffraction state. The formalism allows for a quantitative calculation of the time-dependent photocurrent for moderately correlated systems like simple ferromagnetic metals. A first application to the Fe(100) surface is discussed in detail.
Dokumententyp: | Zeitschriftenartikel |
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Fakultät: | Chemie und Pharmazie > Department Chemie |
Themengebiete: | 500 Naturwissenschaften und Mathematik > 540 Chemie |
ISSN: | 2469-9950 |
Sprache: | Englisch |
Dokumenten ID: | 67567 |
Datum der Veröffentlichung auf Open Access LMU: | 19. Jul. 2019, 12:22 |
Letzte Änderungen: | 04. Nov. 2020, 13:49 |