An ARPES study of correlated electron materials on the verge of cooperative order

In this thesis the charge dynamics of correlated electron systems, in which a metallic phase lies in close proximity to an ordered phase, are investigated by means of angle resolved photoemission spectroscopy (ARPES). The analysis of the experimental data is complemented by electronic structure calculations within the framework of density functional theory (DFT). First the charge dynamics of the colossal magnetoresistant bilayer manganites are studied. The analysis of the ARPES spectra based on DFT calculations and a Peierls type charge density wave model, suggests that charge, orbital, spin and lattice degrees of freedom conspire to form a fluctuating two dimensional local order that produces a large pseudo gap of about 450 meV in the ferromagnetic metallic phase and that reduces the expected bilayer splitting. Next, the interplay of Kondo physics and (magnetic) order in the heavy fermion superconductor URu2Si2 is investigated. The low energy electronic structure undergoes strong changes at 17.5 K, where a second order phase transition occurs whose phenomenology is well characterized, but whose order parameter could not yet be unambigeously identified. Below THO, non-dispersive quasi particles with a large scattering rate suddenly acquire dispersion and start to hybridize with the conduction band electrons. Simultaniously the scattering rate drops sinificantly and a large portion of the Fermi surface vanishes due to the opening of a gap within the band of heavy quasi particles. The observed behaviour is in stark contrast to conventional heavy fermion systems where the onset of hybridization between localized and itinerant carriers happens in a crossover type transition rather than abruptly. These experimental results suggest that Kondo screening and the hidden order parameter work together to produce the unusual thermodynamic signatures observed in this compound. Finally, the influence of charge doping and impurity scattering on the superconducting porperties of the transition metal substituted iron pnictide superconductor Ba(Fe1-xTMx)2As2 (TM = Co, Ni) is studied. Here, resonant soft X-ray ARPES is applied to see element selective the contribution of the 3d states of the TM substitute to the Fe 3d host bands. The spectroscopic signatures of the substitution are found to be well reproduced by DFT supercell and model impurity calculations. Namely, the hybridization of the dopant with the host decreases with increasing impurity potential and the electronic states of the impurtiy become increasingly localized. Simultaniously, in all simulated cases a shift of the Fermi level due to electron doping is observed. The magnitude of the shift in the chemical potential that accurs in BaFe2As2, however, is in stark contrast to the marginal doping values obtained for the impurity model, where the shift of the chemical potential is largely compensated by the influence of the increasing impurity potential. This suggests that the rigid band behaviour of TM substituded BaFe2As2 is a peculiarity of the compound, which has strong implications for the developement of superconductivity.In dieser Arbeit wird die Ladungstraegerdynamik in korrelierten Elektronensystemen, in denen eine metallische Phase in direkter Nachbarschaft zu einer geordneten Phase liegt, mit Hilfe von winkelaufgeloester Photoelektronenspektroskopie (ARPES) untersucht. Die Analyse der experimentellen Daten wird ergaenzt durch lektronenstrukturrechnungen im Rahmen der Dichtefunktionaltheorie (DFT). Zuerst wird die Ladungstraegerdynamik in gemischtvalenten zweischichtmanganaten mit kolossalem Magnetiwiderstand studiert. Die Analyse der Photoemissionsspektren basierend auf DFT Rechnungen und einem Peierls artigem Ladungsdichtewellenmodell, legt nahe, dass die Freiheitsgrade von Ladung, Orbitalen, Spin und des Ionengitters konspirieren, um eine fluktuierende zweidimensionale lokale Ordnung zu bilden, die verantwortlich ist fuer die beobachtete Pseudobandluecke von 450 meV, und die zur Reduktion der erwarteten Zweischichtaufspaltung beitraegt. Als naechstes wird das Zusammenspiel von Kondo Physik und (magnetischer) Ordung im Schwerfermionensupraleiter URu2Si2 untersucht. Die iedrigenergetische elektronische Struktur zeigt starke Veraenderungen bei 17.5 K, wo ein Phasenuebergang zweiter Ordnungstattfindet, der phenomenologisch gut charakterisiert ist, aber dessen Ordungsparameter nocht nicht eindeutig identifiziert werden konnte. Unterhalb von THOerlangen nicht dispergierende Quasiteilchen mit gro en Streuraten abrupt Dispersion und hybridisieren mit den Leitungselektronen. Gleichzeitig sinkt die Streurate und ein gro er Teil der Fermiflaeche verschwindet durch das Oeffnen einer Bandluecke innehalb des Bandes schwerer Quasiteilchen. Das beobachtete Verhalten steht in starkem Kontrast zu dem von konventionellen Schwerfermionensystemen, in denen die Hybridisierung zwischen lokalisierten und itineranten Ladungstraegern in einem kontinuierlichen Uebergang ablaeuft, anstatt abrubt. Diese experimentellen Befunde lassen den Schluss zu, dass das zusammenspiel zwischen Kondo Abschirmung und dem unbekannten Ordnungsparameter die ungewoehnlichen thermodynamischen Signaturen in dieser Verbindung hervorruft. Abschliessend wird das Zusammenwirken von Ladungstraegerdotierung und Streuung an Stoeratomen auf die Supraleitung uebergangsmetalldotierter Eisenpniktid Supraleiter Ba(Fe1-xTMx)2As2 (TM = Co, Ni) untersucht. Mit Hilfe von resonantem Weichenroentgen ARPES gelingt es, elementselektiv den Beitrag der 3d Zustaende des TM Substituenten zu den Eisen 3d Wirtsbaendern zu beobachten. Die spektroskopischen Signaturen der Substitution sind mit Hilfe von DFT Rechnungen und Modelrechnungen mit zufaellig verteilten Stoeratomen gut zu reproduzieren. Insbesondere nimmt die Hybridisierung des dotierten Uebergangsmetalls und der Eisenbaender mit zunehmender Kernladungszahl ab und die elektronischen Zustaende der Stoeratome werden zunehmen lokalisiert. Gleichzeitig wird in allen gerechneten Faellen eine Verschiebung des Fermi Niveaus durch Elektronendotierung beobachtet. Der Betrag der Verschiebung des chemischen Potentials in BaFe2As2 steht allerdings in starkem Kontrast zu den Werten, die man im Falle der Modellrechnungen erhaelt, wo die Verschiebung des Fermi Niveaus durch den Einfluss des Potentials der Stoeratome groesstenteils kompensiert wird. Dies legt nahe, dass das beobachtete "rigid band" Verhalten von TM substituiertem BaFe2As2 eine Besonderheit dieser Verbindung ist, welches starke Auswirkungen auf die Ausbildung von Supraleitung hat

Formation of the coherent heavy fermion liquid at the 'hidden order' transition in URu2Si2

In this article we present high-resolution angle-resolved photoemission (ARPES) spectra of the heavy-fermion superconductor URu$_2$Si$_2$. Measurements as a function of both excitation energy and temperature allow us to disentangle a variety of spectral features, revealing the evolution of the low energy electronic structure across the hidden order transition. Already above the hidden order transition our measurements reveal the existence of weakly dispersive states below the Fermi level that exhibit a large scattering rate. Upon entering the hidden order phase, these states transform into a coherent heavy fermion liquid that hybridizes with the conduction bands.Comment: 5 pages, 4 figure

Stabilization mechanism of molecular orbital crystals in IrTe2

Doped IrTe2 is considered a platform for topological superconductivity and therefore receives currently a lot of interest. In addition, the superconductivity in these materials exists in close vicinity to electronic order and the formation of molecular orbital crystals, which we explore here by means of high-pressure single crystal x-ray diffraction in combination with density functional theory. Our crystallographic refinements provide detailed information about the structural evolution as a function of applied pressure up to 42 GPa. Using this structural information for density functional theory calculations, we show that the local multicenter bonding in IrTe2 is driven by changes in the Ir-Te-Ir bond angle. When the electronic order sets in, this bond angle decreases drastically, leading to a stabilization of a multicenter molecular orbital bond. This unusual local mechanism of bond formation in an itinerant material provides a natural explanation for the different electronic orders in IrTe2. It further illustrates the strong coupling of the electrons with the lattice and is most likely relevant for the superconductivity in this material

Stabilization mechanism of molecular orbital crystals in IrTe2

Doped IrTe2 is considered a platform for topological superconductivity and therefore receives currently a lot of interest. In addition, the superconductivity in these materials exists in close vicinity to electronic order and the formation of molecular orbital crystals, which we explore here by means of high-pressure single crystal x-ray diffraction in combination with density functional theory. Our crystallographic refinements provide detailed information about the structural evolution as a function of applied pressure up to 42 GPa. Using this structural information for density functional theory calculations, we show that the local multicenter bonding in IrTe2 is driven by changes in the Ir-Te-Ir bond angle. When the electronic order sets in, this bond angle decreases drastically, leading to a stabilization of a multicenter molecular orbital bond. This unusual local mechanism of bond formation in an itinerant material provides a natural explanation for the different electronic orders in IrTe2. It further illustrates the strong coupling of the electrons with the lattice and is most likely relevant for the superconductivity in this material