Since the discovery of cuprate superconductors, PrBa2Cu3O7 (Pr123) has attracted much attention due to its nonsuperconductivity and other anomalies. The very recent reports on superconducting Pr123 instead of putting an end of this issue, virtually stimulate more controversies. One of the proposed explanations for the recently observed superconductivity in Pr123 is that the samples could be Ba-rich Pr123 to investigate this possibility, we prepared Pr1-xBa2+xCu3O7 (x=1~0.3) and Pr1-xCaxBa2Cu3O7 (x=0~0.6) as comparison. X-ray absorption near edge spectroscopy (XANES) indicates an increase in carrier concentration with Ba and Ca doping, which is consistent with resistivity and thermoelectric power(TEP) data. However, carriers are introduced in a peculiar why rather than simply add into CuO2 plane.

Thesis advisor: Ziqiang Wang / One of the most unconventional electronic states in high transition temperature cuprate superconductors is the pseudogap state. In the temperature versus doping phase diagram, the pseudogap state straddles across the antiferromagnetic (AF) state near half filling and the superconducting (SC) dome on the hole doped side above the transition temperature Tc. The relationship between the pseudogap state and these two well known states - the AF state and the SC state is believed to be very important for understanding superconductivity and the emergent quantum electronic matter in doped Mott insulators. The pseudogap is characterized by the emergence of a soft gap in the single-particle excitation spectrum in the normal state in the temperature range between Tc and a characteristic temperature T*, i.e. Tc < T < T*. The most puzzling feature of the pseudogap is the nodal-antinodal dichotomy. Observed by ARPES in momentum space, the Fermi surface is gapped out in the antinodal region leaving a Fermi arc of gapless excitations near the nodes. Whether the pseudogap is an incoherent superconducting gap (onegap scenario) or it is a different gap governed by other mechanisms, other than superconductivity, (two-gap scenario) is still under debate. In this thesis I study the particle-particle channel and the particle-hole channel of the valence bond fluctuations away from half filling. Based on a strong-coupling analysis of the t-J model, I argue that the superexchange interaction J induced incommensurate bond centered density wave order is the driving mechanism for the pseudogap state. Low energy density of states (DOS) are eliminated by multiple incommensurate scatterings in the antinodal region at the Fermi level. I show that the interplay between the incommensurate bond centered d-wave density wave instability and the intrinsic electronic inhomogeneity in real cuprate materials is responsible for the observed pseudogap phenomena. Utilizing the spatially unrestricted Gutzwiller approximation, I show that the off-stoichiometric doping induced electrostatic disorder pins the low-energy d-wave bond density fluctuations, resulting in a VBG phase. The antinodal Fermi surface (FS) sections are gapped out, giving rise to a genuine normal state Fermi arc. The length of the Fermi arc shrinks with underdoping below the temperature T* determined by thermal filling of the antinodal pseudogap. Below Tc, the d-wave superconducting gap due to singlet pairing coexists and competes with the VBG pseudogap. The spatial, momentum, temperature and doping dependence of these two gaps are consistent with recent ARPES and STM observations in underdoped and chemically substituted cuprates. The temperature versus doping phase diagram captures the salient properties of the pseudogap phenomena and provides theoretical support for the two-gap scenario. In addition to resolving the complexities of the quantum electronic states in hole-doped cuprates, my unified theory elucidates the important role of the interplay between the strong electronic correlation and the intrinsic electronic disorder in doped transition metal oxides. / Thesis (PhD) — Boston College, 2011. / Submitted to: Boston College. Graduate School of Arts and Sciences. / Discipline: Physics.

京都大学 / 新制・課程博士 / 博士(理学) / 甲第23696号 / 理博第4786号 / 新制||理||1685(附属図書館) / 京都大学大学院理学研究科物理学・宇宙物理学専攻 / (主査)教授 松田 祐司, 教授 柳瀬 陽一, 教授 石田 憲二 / 学位規則第4条第1項該当 / Doctor of Science / Kyoto University / DFAM

In dieser Doktorarbeit wird der Hochtemperatur-Supraleiter Bi-2212 auf seine elektronische Struktur hin untersucht. Für diesen Zweck wurden Röntgen- Absorptionsspektroskopie (XAS) und winkelaufgelöste Photoemissionsspektroskopie (ARPES) verwendet. Zusätzlich wurden mittels Dichtefunktionaltheorie theoretische Trends in der elektronischen Struktur aufgezeigt. Zu Beginn wurde die Temperaturabhängigkeit der Löcher-Konzentration (nH) von nahezu optimal dotierten und geringfügig unterdotierten Einkristallen mittels XAS untersucht. Die Messungen der Temperaturabhängigkeit von nH mit XAS zeigen ein komplett anderes Verhalten als das, welches aus dem Hall-Effekt hergeleitet wurde. Hinzu kommt, dass es unmöglich ist, die Formel von Gor''kov und Teitel''baum, d.h. mit einem konstanten und einem Aktivierungsterm, an die Daten anzupassen. Als Lösungsansatz kommen Magnonen in Frage. Zusätzlich wurde die Polarisationsabhängigkeit der Löcher- Konzentration mittels XAS gemessen, die zeigt, dass in den Kupferoxidschichten die Löcher offenbar offenbar inhomogen verteilt sind. Solch ein Verhalten wird für die isotrope Struktur der Bi-2212-Kristalle nicht erwartet und kann nur schwer erklärt werden. Möglicherweise sind die, die Symmetrie brechenden magnetischen Eigenschaften wie magnetische Streifen die Antwort. Um zusätzliche experimentelle Informationen zu erhalten, wurde darüber hinaus noch die Temperatur- und Polarisationsabhängigkeit der Bi-2212-Einkristalle mittels ARPES studiert. Insbesondere die ''Peak-Dip-Hump''-Emissionsstruktur an der Fermi-Energie wurde gemesssen, die sich am M-Punkt der Brillouin-Zone befindet. Die Ergebnisse zeigen, dass der scharfe Peak nahe der Fermi-Kante eine deutliche Polarisations- und Temperaturabhängigkeit aufweist, welche bei der Pseudolücken-Temperatur T* und nicht bei der Sprungtemperatur TC verschwindet. Die Polarisationsabhängigkeit an den vier M-Punkten der Brillouin-Zone hat gezeigt, dass eine Symmetrieachse im 45°-Winkel zur Cu-O-Cu-Richtung existiert. Dies könnte ebenfalls mit magnetischer Streifenbildung erklärt werden. Des Weiteren wurde das beobachtete Versagen der Dipol-Näherung zur Beschreibung der Spektren bei einer Polarisation senkrecht zur Spiegelebene erörtert. Andererseits ist die Berechnung von Materieleigenschaften mittels der Dichtefunktionaltheorie ein sehr aktiver Bereich der Festkörperphysik geworden. Nachdem meine DFT-Rechnungen auf der Basis des MBJ-Potentials sehr gute Übereinstimmung mit den experimentellen Ergebnissen des ternären Halbleiters ZrSexS2-x und die LiZrSexS2-x –Verbindung erzielt haben, habe ich diese auch zur Unterstützung der experimentellen Supraleiterdaten angewendet. Die elektronischen Eigenschaften von CaCuO2 und des Bi-2212-Kuprats wurden mittels DFT auf der Basis von GGA und GGA+U berechnet, wobei der Hubbard-U-Term mit einer „abinitio“-Methode berechnet wurde. Die Ergebnisse ergaben, dass nur Rechnungen auf der Basis von MBJ+U einen antiferromagnetischen Grundzustand für die CaCuO2- Verbindung lieferten, während alle Funktionale versagten, den antiferromagnetischen Grundzustand für das Bi-2212-Kuprat zu finden. / In this PhD work the electronic structure of high-TC Bi-2212 cuprates is investigated. For this purpose x-ray absorption spectroscopy (XAS) and angle resolved photoemission spectroscopy (ARPES) are used. Additionally, density functional theory is applied for making theoretical trends of the electronic structure evident. At first, the temperature dependence of the hole density (nH) by XAS on nearly optimum and slightly underdoped single crystals is studied. The measurements of the temperature dependence of nH by XAS show completely different behavior as that derived from Hall effect. Moreover, fitting our data by the Gor’kov and Teitel’baum formula, i.e. assuming a constant term and an activation term, was impossible. For solving the problem a contribution of magnons is suggested. Additionally, the polarization dependence of the hole density has been measured by XAS showing that an inhomogeneity of holes in the copper oxide planes may exist. Such a behavior is not expected for the isotropic structure of the Bi(Pb)-2212 crystals and was only hardly to be explained. Possibly, magnetic symmetry breaking properties like e.g. magnetic stripes might give an answer. In order to derive additional experimental information, the temperature and polarization dependence of the electronic structure of the CuO2 planes of Bi(Pb)-2212 single crystals has been studied by ARPES. In particular, the so-called peak-dip-hump emission structure close to the Fermi energy has been measured, which is located at the M point of the Brillouin zone. The results show that the sharp emission structure close to the Fermi edge reveals a distinct polarization dependence and it vanishes at the pseudogap temperature T* and not at the critical temperature TC. The polarization dependence at the four M points of the Brillouin zone has revealed that there exists a symmetry line along to 45?? from the Cu-O-Cu direction. This could also be due to stripe formation. Additionally, the observed failure of the dipole approximation to describe the spectra at normal polarization with respect to the mirror plane is discussed. On the other hand, the calculation of material properties by density functional theory has become a very active area of research in condensed matter physics. Therefore, after my calculations based on DFT by the MBJ potential have revealed good agreement with experimental data for the ternary semiconductors ZrSexS2-x and the LiZrSexS2-x compound I applied it for a support of the experimental superconductor data. The electronic properties of CaCuO2 and the Bi-2212 cuprate have been calculated by DFT based on GGA and GGA+U where the Hubbard U term has been calculated by an ab initio method. The results reveal that only calculations based on MBJ+U lead to an anti-ferromagnetic ground state for the CaCuO2 compound while all functionals fail to find an antiferromagnetic ground state for Bi-2212.

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