@phdthesis{Kissner2022,
  author    = {Kißner, Katharina},
  title     = {Manipulation of electronic properties in strongly correlated Cerium-based surface alloys},
  doi       = {10.25972/OPUS-27306},
  url       = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-273067},
  school      = {Universit{\"a}t W{\"u}rzburg},
  year      = {2022},
  abstract  = {Photoelectron spectroscopy proves as a versatile tool for investigating various aspects of the electronic structure in strongly correlated electron systems. Influencing the manifestation of strong correlation in Ce-based surface alloys is the main task of this work. It is shown, that the manifestation of the Kondo ground state is influenced by a multitude of parameters such as the choice of the metal binding partner in binary Ce compounds, the surface alloy layer thickness and accompanying variations in the lattice structure as well as the interfaces to substrate or vacuum. Gaining access to these parameters allows to directly influence essential state variables, such as the f level occupancy nf or the Kondo temperature TK. The center of this work are the intermetallic thin films of CePt5/Pt(111) and CeAgx/Ag(111). By utilizing different excitation energies, photoemission spectroscopy provides access to characteristic features of Kondo physics in the valence band, such as the Kondo resonance and its spin-orbit partner at the Fermi level, as well as the multiplet structure of the Ce 3d core levels. In this work both approaches are applied to CePt5/Pt(111) to determine nf and TK for a variety of surface alloy layer thicknesses. A temperature dependent study of the Ce 3d core levels allows to determine the systems TK for the different layer thicknesses. This leads to TK ≈200-270K in the thin layer thickness regime and TK >280K for larger layer thicknesses. These results are confirmed by fitting the Ce 3d multiplet based on the Gunnarsson-Sch{\"o}nhammer formalism for core level spectroscopy and additionally by valence band photoemission spectra of the respective Kondo resonances. The influence of varying layer thickness on the manifestation of strong correlation is subsequently studied for the surface alloy CeAgx/Ag(111). Furthermore, the heavy element Bi is added, to investigate the effects of strong spin-orbit coupling on the electronic structure of the surface alloy.},
  subject      = {Korrelation},
  language  = {en}
}
@phdthesis{Praetorius2015,
  author    = {Praetorius, Christian Michael},
  title     = {Ce M4,5 XAS and XMCD as Local Probes for Kondo and Heavy Fermion Materials - A Study of CePt5/Pt(111) Surface Intermetallics -},
  url       = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-132504},
  school      = {Universit{\"a}t W{\"u}rzburg},
  year      = {2015},
  abstract  = {The aim of the present thesis is to explore the potential of X-ray magnetic circular dichroism(XMCD) experiments on gaining new insights into Kondo and heavy fermion materials. XMCD, which is derived from X-ray absorption spectroscopy (XAS), allows probing magnetic polarization specific to the different elements in a material and to their atomic orbitals. In particular, at the Ce M4,5 edges the method is sensitive to the localized 4f level, which provides the magnetic impurity moment responsible for Kondo physics in Ce compounds. Hence, Ce M4,5 XMCD is ideally suited to investigate local magnetism in the presence of interaction of impurity and conduction electrons in such materials. As a model material, CePt5/Pt(111) surface intermetallics were chosen for the present study. This thin-film material can be prepared by well-defined procedures involving molecular beam epitaxy. Crystalline Ordered samples are obtained by exploiting the single-crystallinity of the Pt(111) substrate. The surface character of thin films ideally matches the probing depth of soft X-ray spectroscopy in the total electron yield mode. The XMCD and XAS experiments, taking into account dependence on temperature, angle of incidence, sample thickness and external magnetic field, revealed the presence of four relevant energy scales that influence the magnetic response: 1. The 4f level in CePt5/Pt(111) is subject to significant crystal field (CF) splitting, which leads to reorganization of the six j = 5/2 sublevels. The hexagonal symmetry of the crystal structure conserves mj as a good quantum number. The proposed CF scheme, which is derived from measurements of the paramagnetic susceptibility by XMCD as well as linear dichroism in XAS, consists of nearly degenerate |1/2> and |3/2> doublets with the |5/2> doublet excited by E5/2 = 15 ... 25 meV. 2. Single impurity Kondo interaction significantly couples the magnetic moments of the impurity and conduction electrons. A signature thereof is the f0 -> f1 contribution to Ce M4,5 XAS, the strength of which can be tuned by control of the sample thickness. This finding is in line with the observation of reduced effective 4f moments as detected by XMCD. 3. Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction induces ferromagnetic correlations on the impurity lattice, which induces a positive Curie-Weiss temperature in the temperature-dependent inverse susceptibility. 4. Indications for the transition to a coherent heavy fermion state are found in the inverse susceptibility at T ~ 20 K; the ferromagnetic ground state is not observed. The fielddependence of the magnetic moment in the coherent state can be interpreted in terms of a metamagnetic transition. This allows studying basic characteristics of the renormalized band structure of a heavy fermion system by XMCD. The disentanglement of these different contributions to the 4f magnetism not only required extensive Ce M4,5 XAS and XMCD data, but also a thorough structural characterization of the material, a fundamental study of the Ce M4,5 line shape in relation to the degree of 4f hybridization and the development of a model for the paramagnetic susceptibility. The unit cell dimensions and sample morphology of CePt5/Pt(111) intermetallics were studied by low-energy electron diffraction (LEED) and scanning transmission electron microscopy (STEM). These experiments showed that well-defined intermetallic films form on top of the substrate. This lead to introduction of the film thickness t, measured in unit cells (u.c.), as a key feature to characterize the samples. Systematic LEED measurements in the thickness range t ~ 1 ... 15 u.c. allowed identification of six different phases, which could be interpreted as resulting from the same crystal structure with different rotational alignments and lattice constants. An accurate determination of the surface lattice constant at t ~ 3 u.c. could be achieved by interpretation of additional superstructure spots as arising from a well-defined combination of substrate and film lattices. The thicknessdependence of the lateral lattice constant could be explained in terms of lattice relaxation. Confirmation of the CePt5 stoichiometry and structure was performed by use of thicknessdependent XAS and a representative LEED-IV study. The results of this study indicate that the intermetallic films exhibit hexagonal CaCu5 structure over the entire range of thicknesses that were studied. The terminating layer consists purely of Pt with one additional Pt atom per unit cell compared to the bulk structure. The line shape of Ce M4,5 spectra was analyzed with the help of full multiplet calculations. Experimentally, characteristic variations of the line shape were observed with increasing f0 -> f1 contribution. The calculations show that these variations are not due to an admixture of j = 7/2 character to the ground state, as often stated in the literature. As alternatives, this observation can be explained by either considering an additional contribution to the spectrum or by assumption of an asymmetric lifetime profile. The model that was developed for the inverse paramagnetic susceptibility contains the hexagonal crystal field, magnetic coupling of the impurity moments in a mean field scheme and Kondo screening. The latter is included phenomenologically by screening factors for the effective moment. Assumption of doublet-specific screening factors, which means that the degree of Kondo interaction depends on the mj character of the 4f sublevels, allows satisfactory reproduction of the experimental data.},
  subject      = {Magnetischer R{\"o}ntgenzirkulardichroismus},
  language  = {en}
}
@phdthesis{Klein2009,
  author    = {Klein, Markus},
  title     = {Starke Korrelationen in Festk{\"o}rpern : von lokalisierten zu itineranten Elektronen},
  url       = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-36459},
  school      = {Universit{\"a}t W{\"u}rzburg},
  year      = {2009},
  abstract  = {In dieser Arbeit wurden mittels winkelaufgel{\"o}ster Photoemission verschiedene Verbindungen mit stark korrelierten Elektronen untersucht. Es wurde gezeigt, dass diese Technik einen direkten Zugang zu den niederenergetischen Wechselwirkungen bietet und dadurch wichtige Informationen {\"u}ber die Vielteilchenphysik dieser Systeme liefert. Die direkte Beobachtung der scharfen Quasiteilchenstrukturen in der N{\"a}he der Fermikante erm{\"o}glichte insbesondere die genaue Betrachtung der folgenden Punkte: 1. Quantenphasen{\"u}bergang: analog zu [27] wurde gezeigt, dass die hochaufgel{\"o}ste PES Zugriff auf die lokale Energieskala TK bietet. Außerdem konnte im Rahmen eines st{\"o}rungstheoretischen Modells allgemein gezeigt werden, wie sich kleine RKKY-St{\"o}rungen auf TK auswirken. Aus der experimentellen Entwicklung von TK(x) in CeCu6-xAux lassen sich mit Hilfe dieses Modells R{\"u}ckschl{\"u}sse auf den Quantenphasen{\"u}bergang bei T = 0 ziehen. 2. Kondogitter: mit Hilfe einer geordneten CePt5/Pt(111)-Oberfl{\"a}chenlegierung wurde demonstriert, dass mit ARPES Kondogittereffekte beobachtet werden k{\"o}nnen. Dazu z{\"a}hlen die Beobachtung von Hybridisierungsbandl{\"u}cken und der starken Renormierung der Bandmassen in der N{\"a}he von EF. Diese Effekte lassen sich, mit Hilfe unterschiedlicher Anregungsenergien und Messungen an einer isostrukturellen LaPt5-Schicht, eindeutig dem Resultat einer d f -Mischung der elektronischen Zust{\"a}nde zuweisen. Anhand von temperaturabh{\"a}ngigenMessungen konnte erstmals der {\"U}bergang von lokalisierten zu koh{\"a}renten Quasiteilchen in einem Kondosystem mittels ARPES beobachtet werden. 3. Phasen{\"u}berg{\"a}nge: bei FeSi und URu2Si2 wurde jeweils gezeigt, dass die ARPES sensitiv f{\"u}r kleinste {\"A}nderungen der elektronischen Struktur in unmittelbarer Umgebung der Fermienergie ist. Es konnten charakteristische Energien und Temperaturen, sowie am Phasen{\"u}bergang beteiligte B{\"a}nder und deren effektive Massen m* quantifiziert werden. Insbesondere wurde gezeigt, dass Heavy-Fermion-B{\"a}nder mit m* = 40 me eine wichtige Rolle beim Hidden-order-Phasen{\"u}bergang in URu2Si2 spielen. 4. Oberfl{\"a}cheneffekte: f{\"u}r alle Proben, außer CeCu6-xAux, musste festgestellt werden, dass Oberfl{\"a}chenzust{\"a}nde betr{\"a}chtliche Anteile am Spektrum besitzen k{\"o}nnen. Daher ist bei jedem Material gr{\"o}ßte Vorsicht bei der Pr{\"a}paration der Oberfl{\"a}che und der Interpretation der Spektren angebracht. Als eine geeignete Methode um Oberfl{\"a}chen und Volumenanteile auseinander zu halten, stellten sich anregungsenergieabh{\"a}ngige Messungen heraus. 5. theoretische Modelle: trotz der Bezeichnung "stark korrelierte Systeme", unterscheiden sich die untersuchten Verbindungen bez{\"u}glich ihrer theoretischen Beschreibung: die Physik der Cersysteme (CeCu6, CePt5/Pt(111)) ist bei T > TK durch lokale St{\"o}rstellen bestimmt und lassen sich somit im Rahmen des SIAM beschreiben. Bei tieferen Temperaturen T < TK treten jedoch Anzeichen von beginnender Koh{\"a}renz auf und geben somit den {\"U}bergang zum PAM wieder. Schwere, dispergierenden B{\"a}nder in URu2Si2 und FeSi zeigen, dass beide Systeme nur mit Hilfe eines geordneten Gitters beschreibbar sind. Insbesondere stellt sich f{\"u}r FeSi heraus, dass eine Erkl{\"a}rung im Kondoisolator-Bild falsch ist und ein Hubbard-Modell-Ansatz angebrachter scheint.},
  subject      = {Kondo-Effekt},
  language  = {de}
}