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  • About
  • The Global ETD Search service is a free service for researchers to find electronic theses and dissertations. This service is provided by the Networked Digital Library of Theses and Dissertations.
    Our metadata is collected from universities around the world. If you manage a university/consortium/country archive and want to be added, details can be found on the NDLTD website.
21

Correlated low temperature states of YFe2Ge2 and pressure metallised NiS2

Semeniuk, Konstantin January 2018 (has links)
While the free electron model can often be surprisingly successful in describing properties of solids, there are plenty of materials in which interactions between electrons are too significant to be neglected. These strongly correlated systems sometimes exhibit rather unexpected, unusual and useful phenomena, understanding of which is one of the aims of condensed matter physics. Heat capacity measurements of paramagnetic YFe$_{2}$Ge$_{2}$ give a Sommerfeld coefficient of about 100 mJ mol$^{−1}$ K$^{−2}$, which is about an order of magnitude higher than the value predicted by band structure calculations. This suggests the existence of strong electronic correlations in the compound, potentially due to proximity to an antiferromagnetic quantum critical point (QCP). Existence of the latter is also indicated by the non-Fermi liquid T$^{3/2}$ behaviour of the low temperature resistivity. Below 1.8 K a superconducting phase develops in the material, making it a rare case of a non-pnictide and non-chalcogenide iron based superconductor with the 1-2-2 structure. This thesis describes growth and study of a new generation of high quality YFe$_{2}$Ge$_{2}$ samples with residual resistance ratios reaching 200. Measurements of resistivity, heat capacity and magnetic susceptibility confirm the intrinsic and bulk character of the superconductivity, which is also argued to be of an unconventional nature. In order to test the hypothesis of the nearby QCP, resistance measurements under high pressure of up to 35 kbar have been conducted. Pressure dependence of the critical temperature of the superconductivity has been found to be rather weak. μSR measurements have been performed, but provided limited information due to sample inhomogeneity resulting in a broad distribution of the critical temperature. While the superconductivity is the result of an effective attraction between electrons, under different circumstances the electronic properties of a system can instead be dictated by the Coulomb repulsion. This is the case for another transition metal based compound NiS$_{2}$, which is a Mott insulator. Applying hydrostatic pressure of about 30 kbar brings the material across the Mott metal-insulator transition (MIT) into the metallic phase. We have used the tunnel diode oscillator (TDO) technique to measure quantum oscillations in the metallised state of NiS$_{2}$, making it possible to track the evolution of the principal Fermi surface and the associated effective mass as a function of pressure. New results are presented which access a wider pressure range than previous studies and provide strong evidence that the effective carrier mass diverges close to the Mott MIT, as expected within the Brinkman-Rice scenario and predicted in dynamical mean field theory calculations. Quantum oscillations have been measured at pressures as close to the insulating phase as 33 kbar and as high as 97 kbar. In addition to providing a valuable insight into the mechanism of the Mott MIT, this study has also demonstrated the potential of the TDO technique for studying materials at high pressures.
22

Evolução da superfície de Fermi do La2-xSrxCuO4: estados locais de Wannier/Hartree-Fock

VIELZA DE LA CRUZ, Yoandris 30 August 2016 (has links)
Submitted by Irene Nascimento (irene.kessia@ufpe.br) on 2017-04-17T18:48:07Z No. of bitstreams: 2 license_rdf: 1232 bytes, checksum: 66e71c371cc565284e70f40736c94386 (MD5) Dissertação Mestrado.pdf: 3421668 bytes, checksum: 4a6d6f2568841028e0b66b952f2d15ba (MD5) / Made available in DSpace on 2017-04-17T18:48:07Z (GMT). No. of bitstreams: 2 license_rdf: 1232 bytes, checksum: 66e71c371cc565284e70f40736c94386 (MD5) Dissertação Mestrado.pdf: 3421668 bytes, checksum: 4a6d6f2568841028e0b66b952f2d15ba (MD5) Previous issue date: 2016-08-30 / Este trabalho é uma extensão de uma modelagem tight−binding de estados de Wannier com interação coulombiana de screening para a descrição de elétrons correlacionados nas camadas de CuO2 do La2CuO4. Na condição de banda semicheia e temperatura T = 0 K, esta modelagem é capaz de predizer um estado fundamental antiferromagnético isolante e um estado excitado paramagnético com pseudo-gap, cuja natureza ainda é debatido na literatura. Esses estados são obtidos no contexto de uma solução auto-consistente tipo Hartree-Fock na modelagem de uma banda efetiva de estados de Wannier, sob condições de quebra de simetria de translações espaciais e efeito de emaranhamento (entanglement) na estrutura espinorial dos estados eletrônicos. No regime dopado com buracos, esses estados ficam degenerados num ponto crítico de concentração de buracos igual a xc = 0.2, resultando em uma transição de fase quântica de segunda ordem para um estado paramagnético. A modelagem dá assim explicação à existência detectada experimentalmente desta transição de fase. Em nosso trabalho generalizamos o termo cinético da modelagem acima mencionada através da inclusão de hopping entre segundos vizinhos, de acordo com observações experimentais. De fato, a inclusão deste novo termo cinético resulta em melhor concordância da previsão da modelagem e as observações experimentais da evolução da superfície de Fermi com dopagem de buracos. Em particular, enquanto na modelagem restrita a primeiros vizinhos não podemos conciliar a transição de fase quântica observada a xc = 0.2 com as características experimentais da evolução da superfície de Fermi, isto torna-se possível com a inclusão do hopping de segundos vizinhos com amplitude sugerida pelos resultados experimentais. / This work is an extension of a tight - binding model of states of Wannier with screened Coulomb interaction to the description of correlated electrons in the layers of CuO2 of the La2CuO4. In condition of half-filled band and temperature T = 0 K, this model is able to predict a antiferromagnetic insulating ground state and a paramagnetic excited state with pseudo-gap, which nature is still debated in the literature. These states are obtained in the context of a self-consistent solution type Hartree-Fock in the model of an effective band of the Wannier states under breaking conditions of symmetry of space translations and entanglement effect in the spinor structure of the electronic states. In scheme doped with holes, these states are degenerate at critical point of hole concentration equal to xc = 0.2, resulting in a quantum phase transition of second order to paramagnetic state. The model thus gives explanation to the existence of this experimentally detected phase transition. In our work we generalize the kinetic term of above mentioned model by inclusion of hopping between seconds neighboring, according to experimental observations. In fact, the inclusion of this new kinetic term results in better agreement of the forecast of the model and experimental observations of the evolution of the Fermi surface with holes doping. In particular, while the model is restricted to the first neighbors can not reconcile quantum phase transition observed at xc = 0.2 with the experimental characteristics of the evolution of the Fermi surface, this becomes possible with the inclusion of hopping between second neighboring with ampliude suggested by experimental results.
23

Lifshitz transitions in RCo5 (R=Y, La) and in Osmium

Koudela, Daniela 20 February 2007 (has links)
The aim of this thesis was to find anomalies of elastic properties induced by topological changes of the Fermi surface. The latter are called "Lifshitz transitions". Lifshitz transitions are an interesting subject to study because a topological change of the Fermi surface results in a van Hove singularity of the density of states at the Fermi energy, which again induces an anomaly in the free energy and therefore yield anomalies of observable physical quantities. In all cases the question arose, if the corresponding van Hove singularities are large enough to cause anomalies in the elastic properties, which are measurable by nowadays experimental techniques and computable within the accuracy reachable in nowadays computer calculations. The calculations have been done with the Full-Potential nonorthogonal Local-Orbital minimum-basis band-structure code FPLO. To shift the van Hove singularities through the Fermi energy we used hydrostatic pressure, which is mimicked in the computations by decreasing the volume of the unit cell. The materials under consideration had been YCo5 and LaCo5 as examples for magnetic compounds and the element Osmium as an example for a non-magnetic material. All these materials exhibit hexagonal symmetry. In the case of YCo5 our calculations yield a first order Lifshitz transition. Here, an extraordinarily large peak in the spin-up part of the DOS, which is caused by a nearly dispersionless band in the hexagonal plane, crosses the Fermi level under a pressure of about 21 GPa. Thus, the spin-up 3d states become partly depopulated, which results in a drop of the total magnetic moment of 35%. Therefore the transition can be regarded as a transition from strong to weak ferromagnetism. Further, the transition results in a volume collapse of 1.4%. Though the volume collapse is isomorphic, it exhibits the following anisotropy: while the lattice constant in the hexagonal plane is almost smoothly contracting with increasing pressure, the lattice constant in c-direction collapses at the transition-pressure. This volume collapse has been verified in experiment. Analogous calculations have been performed for the compound LaCo5, which is isoelectronic to YCo5. Here as well we predict a first order Lifshitz transition, taking place at a pressure of about 23 GPa. The mechanism of the transition is the same than in YCo5. Again we find a volume collapse under pressure together with a decrease of the magnetic moment. The relative volume change amounts to 1.3%. Like in YCo5, the unit cell dimensions in the hexagonal plane are decreasing almost smoothly with pressure while in c-direction the lattice constant collapses at the transition-pressure. For LaCo5 there are no such experiments done so far to the best of our knowledge. For Osmium we found, that LDA reproduces the ground state volume very well. Furthermore, we could detect three Lifshitz transitions taking place at very high pressures of about 72 GPa, 81 GPa, and 122 GPa. At first, a hole ellipsoid appears at the Gamma-point (V=24.6Å^3, P=72 GPa), then a neck is created at the symmetry-line LH (V=24.2Å^3, P=81 GPa), and finally a hole ellipsoid appears at the L-point (V=23.2 Å^3, P=122 GPa). Due to a degeneracy in the band structure, the hole ellipsoid at the L-point appears at the same pressure when the necks, situated at the symmetry-lines LH merge at L. The corresponding van Hove singularities in the DOS are very tiny and thus no anomalies in the elastic properties could be detected. Furthermore, we showed that the kink in c/a at 25 GPa and at 27 GPa found by Occelli et al. [Occelli et al., Phys. Rev. Lett. 93, 095502 (2004)] and Ma et al. [Ma et al., Phys. Rev. B 72, 174103 (2005)], respectively, is not statistically significant and that (c/a)(P) can be fitted equally well by a smooth function as by piece-wise linear functions as proposed in these references. / Das Ziel dieser Arbeit war es, Anomalien in den elastischen Eigenschaften zu finden, die durch topologische Änderungen der Fermifläche - genannt "Lifschitz Übergänge" - hervorgerufen werden. Lifschitz Übergänge sind ein interessantes Forschungsgebiet, denn die topologische Änderung der Fermifläche führt zu einer van Hove Singularität in der Zustandsdichte, die an der Fermienergie liegt und eine Anomalie in der freien Energie hervorruft und deswegen zu Anomalien in beobachtbaren physikalischen Größen führt. In allen Fällen kam die Frage auf, ob die entsprechenden van Hove Singularitäten groß genug sind, um mit heutigen Methoden meßbare und berechenbare Anomalien in den elastischen Eigenschaften zu verursachen. Die Daten wurden mit dem Computerprogramm FPLO (Full-Potential nonorthogonal Local-Orbital minimum-basis band-structure scheme) berechnet. Um die van Hove Singularitäten durch die Fermienergie zu schieben, verkleinerten wir das Volumen der Einheitszelle, um hydrostatischen Druck zu simulieren. Als zu untersuchende Stoffe wurden YCo5 und LaCo5 als Beispiele für magnetische Verbindungen gewählt und Osmium als Beispiel für ein nicht magnetisches Element. Im Falle von YCo5 fanden wir einen Lifschitz Übergang erster Ordnung. Hier springt ein besonders großer Peak im Spin-auf Teil der Zustandsdichte unter einem Druck von ca. 21 GPa über die Fermienergie. Dadurch werden die Spin-auf 3d Zustände teilweise unbesetzt und das magnetische Moment verringert sich um 35%. Deswegen kann man den Übergang als einen Übergang von starkem Ferromagnetismus zu schwachem Ferromagnetismus bezeichnen. Das Volumen verkleinert sich hierbei um 1.4%. Obwohl dieser Volumenkollaps isomorph ist, zeigt er folgende Anisotropie: während die Gitterkonstante in der hexagonalen Ebene mit zunehmendem Druck mehr oder weniger glatt kontrahiert, kollabiert am Übergangsdruck die Gitterkonstante in c-Richtung. Dieser Volumenkollaps wurde vom Experiment verifiziert. Analoge Rechnungen wurden für die Verbindung LaCo5, die isoelektronisch zu YCo5 ist, durchgeführt. Auch hier sagen wir einen Lifschitz Übergang erster Ordnung voraus, der bei einem Druck von ca. 23 GPa stattfinden wird. Der Mechanismus dieses Übergangs ist der selbe wie in YCo5. Wiederum finden wir einen Volumenkollaps unter Druck zusammen mit einer Verringerung des magnetischen Moments. Die relative Volumenänderung beträgt hier 1.3%. Wie in YCo5 verläuft hier die Kontraktion der Gitterkonstante in der hexagonalen Ebene mehr oder weniger glatt, während die Gitterkonstante in c-Richtung am Übergang kollabiert. Für LaCo5 existieren unseres Wissens hierzu noch keine Experimente. Im Falle von Osmium fanden wir drei Lifschitz Übergänge bei sehr hohen Drücken von ca. 72 GPa, 81 GPa, und 122 GPa. Zuerst bildet sich ein Lochellipsoid am Gamma-Punkt (V=24.6Å^3, P=72 GPa), dann bildet sich ein Hals an der Symmetrielinie LH (V=24.2Å^3, P=81 GPa), und zum Schluß erscheint ein Lochellipsoid am L-Punkt (V=23.2 Å^3, P=122 GPa). Auf Grund einer Entartung in der Bandstruktur taucht das Lochellipsoid am L-Punkt an dem Druck auf, an dem sich auch die Hälse auf der Symmetrielinie LH bei L verbinden. Die entsprechenden van Hove Singularitäten in der Zustandsdichte sind jedoch extrem klein und deswegen können keine Anomalien in den elastischen Eigenschaften detektiert werden. Desweiteren zeigten wir, daß der Knick in c/a, den Occelli et al. [Occelli et al., Phys. Rev. Lett. 93, 095502 (2004)] bei 25 GPa und Ma et al. [Ma et al., Phys. Rev. B 72, 174103 (2005)] bei 27 GPa fanden, statistisch nicht relevant ist und daß (c/a)(P) genauso gut von einer glatten Funktion gefittet wird als von stückweise linearen Funktionen.
24

Accurate Band Energies of Metals with Quadratic Integration

Jorgensen, Jeremy John 18 April 2022 (has links)
Materials play an important role in society. Historically, and even at present, materials have been discovered by trial and error, and many of the most useful materials have been discovered by chance. The high-throughput approach aims to remove (as much as possible) chance and guesswork at the experimental level by filtering out materials candidates that are not predicted to exist. Many successes have been recorded. In the high-throughput approach to materials discovery, machined-learned models of materials are created from databases of theoretical materials. These databases are the result of millions of density-functional-theory (DFT) simulations. The size and accuracy of the data in the databases (and, consequently, the predictions of machined-learned models) are most affected by the band energy calculation; most of the computation of a DFT simulation is computing the band energy in the self-consistency cycle, and most of the error in the simulation comes from band energy error. The band energy is obtained from a two-part multidimensional numerical integral over the Brillouin or irreducible Brillouin zone. A quadratic approximation and integration algorithm for computing the band energy in 2D and 3D is described. Analytic and semi-analytic integration of quadratic polynomials over simplices improves the accuracy and efficiency of the calculation. A method is proposed for estimating the error bounds of the quadratic approximation that does not require additional eigenvalues. Error propagation of approximation errors leads to an adaptive refinement approach that is driven by band energy error. Because adaptive meshes have little symmetry, integration is performed within the irreducible Brillouin zone, and a general algorithm for computing the irreducible Brillouin zone is described. The efficiency of quadratic integration is tested on realistic empirical pseudopotentials. When compared to current integration methods, uniform quadratic integration over the irreducible Brillouin zone sometimes results in fewer k-points for a given accuracy. Adaptive refinement fails to improve integration performance because band energy error bounds are inaccurate, especially at accidental crossings at the Fermi level.
25

Die Fermifläche des Kupratsupraleiters Bi2Sr2CaCu2O8+[delta] : Ergebnisse der winkelaufgelösten Photoemissionsspektroskopie

Legner, Sibylle 23 October 2003 (has links)
Das Forschungsgebiet der Kuprat- oder Hochtemperatursupraleiter (HTSL) ist bis heute einer der lebendigsten Bereiche der Physik kondensierter Materie. Ein besonderer Stellenwert kommt dem normalleitenden Zustand oberhalb TC zu, dessen Verständnis wesentlich zu einer Theorie der Hochtemperatur-Supraleitung beitragen könnte. Gegenstand dieser Arbeit ist die Untersuchung der Elektronenstruktur von HTSLn der Bi2Sr2CaCu2O8+[delta](Bi2212)-Familie nahe der Fermifläche im normalleitenden Zustand. Die Experimente wurden mittels winkelaufgelöster Photoemissionsspektroskopie (ARPES) durchgeführt, wobei die hohe Auflösung in Energie und Impuls recht genaue Rückschlüsse auf die Spektralfunktion und die Übergangs-Matrixelemente erlaubt. Die wichtigsten experimentellen Ergebnisse sind: 1) Hochaufgelöste ARPES-Fermiflächenkarten von Bi2212 und (Pb,Bi)2212 zeigen folgendes Bild: Die Hauptfermifläche ist lochartig und um die Ecken der Brillouinzone zentriert. Weiterer Bestandteil der Elektronenstruktur ist die Schattenfermifläche. Bei reinem Bi2212 treten außerdem extrinsische Beugungskopien der Fermifläche auf. 2) ARPES-Messungen entlang der -M-Richtung von Bi2212 zeigen eine starke Abhängigkeit von der Anregungsenergie, die auf starken Matrixelement-Effekten beruht. Verschiedene Methoden zur Bestimmung von kF zeigen, dass die Daten konsistent mit einer lochartigen Topologie der Hauptfermifläche sind. Des Weiteren wird die Qualität verschiedener Methoden zur Bestimmung von kF bei starken Matrixelement-Effekten bewertet. 3) Die Hauptfermifläche von (Pb,Bi)2212 behält ihre lochartige Topologie über einen großen Dotierungsbereich nahe optimaler Dotierung. 4) Erste hochaufgelöste ARPES-Messungen des Zirkulardichroismus wurden an (Pb,Bi)2212 durchgeführt. In der verwendeten nicht-chiralen Messanordnung wird ein CDAD (Circular Dichroism in the Angular Distribution of Photoelectrons)-Effekt beobachtet, dessen Asymmetrie antisymmetrisch bezüglich der Zweischicht-aufgespaltenen Zustände ist.
26

Electronic States of Heavy Fermion Metals in High Magnetic Fields

Rourke, Patrick Michael Carl 25 September 2009 (has links)
Heavy fermion metals often exhibit novel electronic states at low temperatures, due to competing interactions and energy scales. In order to characterize these states, precise determination of material electronic properties, such as the Fermi surface topology, is necessary. Magnetic field is a particularly powerful tool, since it can be used as both a tuning parameter and probe of the fundamental physics of heavy fermion compounds. In CePb3, I measured magnetoresistance and torque for 23 mK ≤ T ≤ 400 mK, 0 T ≤ H ≤ 18 T, and magnetic field rotated between the (100), (110), and (111) directions. For H||(111), my magnetoresistance results show a decreasing Fermi liquid temperature range near Hc, and a T^2 coefficient that diverges as A(H) ∝ |H −Hc|^−α, with Hc ~ 6 T and α ~ 1. The torque exhibits a complicated dependence on magnetic field strength and angle. By comparison to numerical spin models, I find that the “spin-flop” scenario previously thought to describe the physics of CePb3 does not provide a good explanation of the experimental results. Using novel data acquisition software that exceeds the capabilities of a traditional measurement set-up, I measured de Haas–van Alphen oscillations in YbRh2Si2 for 30 mK ≤ T ≤ 600 mK, 8 T ≤ H ≤ 16 T, and magnetic field rotated between the (100), (110), and (001) directions. The measured frequencies smoothly increase as the field is decreased through H0 ≈ 10 T. I compared my measurements to 4f-itinerant and 4f-localized electronic structure calculations, using a new algorithm for extracting quantum oscillation information from calculated band energies, and conclude that the Yb 4f quasi-hole remains itinerant over the entire measured field range, with the behaviour at H0 caused by a Fermi surface Lifshitz transition. My measurements are the first to directly track the Fermi surface of YbRh2Si2 across this field range, and rule out the 4f localization transition/crossover that was previously proposed to occur at H0.
27

Studies of crystalline organic molecular materials under extreme conditions

Biggs, Timothy James January 2006 (has links)
This thesis describes investigations into the properties of -phase BEDT-TTF charge transfer salts. Charge transfer salts are mainly studied as they are very useful test beds for fundamental physics due to the tuneability of their proper- ties and ground states. The effects of temperature and pressure on such systems have been studied, as these allow access to a wide range of different states and properties. Transport properties of these systems have been studied to obtain information about the Fermi surface and effective mass, and the effect of deuter- ation and also change of pressure media will be discussed. The interaction of infrared radiation with these systems has also been investigated and simultaneous pressure and temperature measurements will be presented, something not greatly studied due to the large technical challenges. The techniques and approaches for overcoming these are also discussed. Chapter 1 provides an introduction to the organic materials themselves with particular emphasis on the actual compounds studied. Chapter 2 provides the necessary theoretical background for studying organic charge transfer salts using magnetic quantum oscillations and their infrared re- ectivity. Chapter 3 covers the experimental techniques and also discusses some of the challenges encountered and their solutions to aid others working in this area. Chapter 4 describes an investigation into the transport properties of - (ET)2Cu(SCN)2 by studying Shubnikov-de Haas oscillations using both deuter- ated and normal samples and using two different pressure media, and comparing it to work done using a third. Chapter 5 presents an investigation into the pressure dependence of selected phonon modes in -(ET)2Cu(SCN)2 using infrared radiation on a deuterated sam- ple. Chapter 6 presents what is believed to be the first pressure and temperature dependent infrared study of an organic molecular material. In this case the or- ganic molecular material is d8--(ET)2Cu[N(CN)2]Br, but the techniques should be readily transferable to other materials.
28

Electronic States of Heavy Fermion Metals in High Magnetic Fields

Rourke, Patrick Michael Carl 25 September 2009 (has links)
Heavy fermion metals often exhibit novel electronic states at low temperatures, due to competing interactions and energy scales. In order to characterize these states, precise determination of material electronic properties, such as the Fermi surface topology, is necessary. Magnetic field is a particularly powerful tool, since it can be used as both a tuning parameter and probe of the fundamental physics of heavy fermion compounds. In CePb3, I measured magnetoresistance and torque for 23 mK ≤ T ≤ 400 mK, 0 T ≤ H ≤ 18 T, and magnetic field rotated between the (100), (110), and (111) directions. For H||(111), my magnetoresistance results show a decreasing Fermi liquid temperature range near Hc, and a T^2 coefficient that diverges as A(H) ∝ |H −Hc|^−α, with Hc ~ 6 T and α ~ 1. The torque exhibits a complicated dependence on magnetic field strength and angle. By comparison to numerical spin models, I find that the “spin-flop” scenario previously thought to describe the physics of CePb3 does not provide a good explanation of the experimental results. Using novel data acquisition software that exceeds the capabilities of a traditional measurement set-up, I measured de Haas–van Alphen oscillations in YbRh2Si2 for 30 mK ≤ T ≤ 600 mK, 8 T ≤ H ≤ 16 T, and magnetic field rotated between the (100), (110), and (001) directions. The measured frequencies smoothly increase as the field is decreased through H0 ≈ 10 T. I compared my measurements to 4f-itinerant and 4f-localized electronic structure calculations, using a new algorithm for extracting quantum oscillation information from calculated band energies, and conclude that the Yb 4f quasi-hole remains itinerant over the entire measured field range, with the behaviour at H0 caused by a Fermi surface Lifshitz transition. My measurements are the first to directly track the Fermi surface of YbRh2Si2 across this field range, and rule out the 4f localization transition/crossover that was previously proposed to occur at H0.
29

Characterization of the electronic properties of LaIrIn5: calculations, transport-, heat capacity- and de Haas-van Alphen-experiments / Bestimmung der elektronischen Eigenschaften von LaIrIn5: Rechnungen, Transport-, Wärmekapazitäts- und de Haas-van Alphen-Experimente

Forzani, Eugenio Angelo 12 January 2007 (has links)
No description available.

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