In this thesis, we study stripe states in underdoped cuprate superconductors using the Bogoliubov-de Gennes (BdG) method with appropriate models. In non-self-consistent calculations, the nature of stripe states with coexisting unidirectional Pair Density Wave (PDW), Charge Density Wave (CDW), and Spin Density Wave(SDW) order is studied, and it was found that among these coexisting stripe orders, the SDW order plays a key role in reconstructing the Fermi Surface (FS), and the magnitude of SDW order needs to be relatively small in order for Fermi arcs to be realized, while strong SDW order necessarily leads to completely gapped spectra. In self-consistent calculations, we mapped out parameter regions where stripe SC states can be stabilized, which are in qualitative agreement with the generic phase diagram of cuprate superconductors. In addition, self-consistent PDW solutions with small SDW order are stabilized in some parameter region, forming small FS pockets in antinodal regions. This parameter region is a promising one to explore in future work, where self-consistent BdG calculation is to be carried out with a magnetic field in order to study the effect of magnetic field on the stability of stripes along with the possible quantum oscillations. / Thesis / Master of Science (MSc)

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Condensed matter physics is a rapidly evolving field of research enriched with the synthesis of new materials exhibiting a bewildering variety of phenomena and advances in experimental techniques. Over the years, discoveries and innovations in electronic systems have emphasized the crucial role played by correlations among electrons behind many of the observed unusual properties and have posed serious challenges to the physics community by exposing the lack of well-controlled theoretical methods to study the class of materials known as strongly correlated electronic systems. In these systems, known theoretical techniques typically fail to capture the essential features of the many-body ground state and finite temperature properties of the systems as typical electronic interaction energies are of order of or larger than the kinetic energies. The study of strongly correlated electronic systems went through a revolution in the 1980s and 1990s after the discovery of superconductivity inorganic compounds, in heavy fermion systems and ultimately in copper oxides, referred to as cuprates, by Bednorz and Muller. In particular, the pursuit of understanding the mysterious origin of superconductivity in the cuprates and other associated strange phenomena has fascinated the condensed matter community over last two and half decades leading to most of the important unsolved, and probably interconnected, problems of quantum condensed matter physics such as the metal-insulator transition in low dimensions breakdown of Fermi liquid theory, the origin and behavior of unconventional superconductivity, quantum critical points, electronic in homogeneities and localization in interacting systems. This thesis is devoted to the study of some of the aspects of high-temperature superconductivity and associated phenomena in cuprates. In what follows, I give an overview of the organization of the thesis in to different chapters and their contents. For setting up the stage, in Chapter 1, I give a brief account of some of the remarkable phenomena and properties observed in strongly correlated electronic matter and their salient features, that continue to draw much attention and excitement in current times. The peculiarity of the state of affairs in these systems is emphasized and motivated in the background of the paradigmatic Landau Fermi liquid theory and Hubbard model, the minimal model that is expected to capture the quintessence of electronic strong correlation. In Chapter 2, starting with a brief historical account of the discovery of superconductivity in cuprates, the crystal structure of these materials, their chemical realities and basic electronic details are reviewed. This is followed by a survey of the phase diagram of cuprates, doped with, say, x number of holes per copper site, and a plethora of experimental findings that constitute the high-c puzzle. Characteristics of various observed phases, such as the superconducting, pseudo gap and strange metal phases, are discussed on the basis off acts accumulated through various experimental probes, e.g. nuclear magnetic resonance(NMR), neutron scattering, specific heat, transport and optical conductivity measurements as well as photo emission, tunnelling and Raman spectroscopies. As elucidated, these experiments point toward the need for an unconventional mechanism of superconductivity in cuprates and, more so, for the description of the rather abnormal high-temperature normal state that is realized above the superconducting transition temperature c. Keeping in mind the fact that there is no consensus even about the minimal microscopic electronic model, I review two models, namely the three band model and the t - J model; various approximate treatments of these models have dominated the theoretical developments in this field. A large number of theoretical pictures have been proposed based on different microscopic, semi-microscopic and phenomenological approaches in the past two decades for explaining the genesis of the observed strange phenomena in high-c cuprates. I include brief discussions on only a few of them while citing relevant references. As mentioned above, a variety of approximate microscopic theories, based on both strong and weak coupling approaches, as well as numerical techniques have been tried to understand the cuprate phase diagram and capture the aspects of strong correlations in-built in Hubbard and t -J models. On the other hand, in conventional superconductors and, in general, for the study of phase transitions, phenomenological Ginzburg-Landau(GL) functionals written down from very general symmetry grounds have provided useful description for a variety of systems. Specially, Ginzburg-Landau theory has been proven to be complementary to the BCS theory for attacking a plethora of situations in superconductors, e.g., in homogeneities, structures of an isolated vortex and the vortex lattice etc. The GL functional has found wide applicability for the study of vortex matter in high-c superconductors as well. Inspired by the success of this type of phenomenological route, we propose and develop in Chapter 3 an approach, analogous in spirit to that of Ginzburg and Landau, for the superconducting and pseudogap phases of cuprates. We encompass a large number of well known phenomenologies of cuprate superconductivity in the form of a low-energy effective lattice functional of complex spin-singlet pair amplitudes with magnitude Δm and phase m, i.e. m =Δm exp(i m), that resides on the Cu-Cubonds(indexed by m)of the CuO2 planes of cuprates. The functional respects general symmetry requirements, e.g. the -wave symmetry of the superconducting order parameter as found in experiments. The assumptions and the specific physical picture behind such an approach as well as the key empirical inputs that go into it are discussed in this chapter. We calculate the superconducting transition temperature c and the average magnitude of the local pair amplitude, Δ= (Δm), using single-site mean-field theory for the model. We show that this approximation leads to general features of the doping-temperature(x - T )phase diagram in agreement with experiment. In particular, we find a phase coherent superconducting state with d-wave symmetry below a parabolic Tc (x) dome and a phase incoherent state with a perceptible local gap that persists up to a temperature around which can be thought of as a measure of the pseudogap temperature scale T* . Further, effects of thermal fluctuations beyond the mean-field level are captured via Monte Carlo(MC) simulations of the model for a finite two-dimensional (2D) lattice. We exhibit results for Tc obtained from MC simulations as well as that estimated in a cluster mean field approximation. Based on our picture we remark on contrasting scenarios proposed for the doping dependence of the pseudogap temperature. Chapter 4 describes fluctuation phenomena related to pairing degrees of freedom and manifestations of these effects in various quantities of interest, e.g. superfluid density, specific heat etc., at finite temperature. Fluctuation effects have been studied in detail in superconductors over the years and pursued mainly using either the conventional GL functional or the BCS-framework at a microscopic level. However, the picture, in which the pseudogap phase is viewed as one consisting of bond-pairs with a d-wave symmetry correlation length growing as T approaches Tc, implies fluctuation phenomena of quite a different kind, as we discuss here. The contribution of the bond-pair degrees of freedom to thermal properties is obtained here from the lattice free-energy functional using MC simulation, as mentioned in the preceding paragraph. The results for the superfluid density or superfluid stiffness ps, a quantity measured e.g. via the penetration depth, are discussed. As shown, its doping and temperature dependence compare well with experimental results. In this chapter, I also report the calculation of the fluctuation specific heat Cv(T) and find that there are two peaks in its temperature dependence, a sharp one connected with Tc (ordering of the phase of m)and a relatively broad one(hump)connected to T* (rapid growth of the magnitude of Δm). The former is specially sensitive to the presence of a magnetic field, as we find in agreement with experiment. Vortices are relevant excitations in a superconductor and, in particular, in 2D orquasi-2D systems vortices influence the finite temperature properties in a major way. The results for the temperature dependence of vortex density obtained in the MC simulation of the GL-like model are also mentioned in Chapter 4. I report an estimate of the correlation length as well. These results might have relevance for the large Nernst signal observed over a broad temperature range above c in cuprates, as pointed out there. Properties of an isolated vortex and collective effects arising due to interaction between vortices are of much significance for understanding mixed state of type-II superconductors and thus of cuprates. The superconducting order is destroyed in the core region around the centre of a vortex and the vortex core carries signatures of the normal state in a temperature regime where it is generally unattainable due to occurrence of superconductivity. As mentioned in Chapter 5, vortex properties(e.g. electronic excitation spectrum at the vortex core) in BCS superconductors have been explored theoretically, at a microscopic level through the Bogoliubov-deGennes(BdG) theory as well as using the Ginzburg-Landau functional. However, properties of vortices in cuprate superconductors have been found to be much more unusual than could possibly be captured by straightforward extensions of BCS theory to a -wave symmetry case. Chapter 5 briefly reviews the experimental findings on vortices in the superconducting state of cuprates, mainly as probed by Scanning Tunnelling Microscopy(STM) as well as from other probes such as NMR, neutron scattering, SR etc. I discuss some of the consequences of our GL-like functional regarding vortex properties, namely that of the vortex core and the region around it. We use our model to find Δm and m at different sites m for a 2π vortex whose core is at the midpoint of a square plaquette of Cu lattice sites. The vortex is found to change character from being primarily a phase or Josephson vortex for small x to a more BCS-like or Abrikosov vortex with a large diminution in the magnitude Δm as one approaches the vortex core, for large . Here I do not make any direct comparison with experimental data but discuss implications of our results in the background of existing experimental facts. Unravelling the mysteries of high-Tc cuprates should necessarily involve the understanding of electronic excitations over a broad regime of doping and temperature encompassing the pseudo gap, superconducting and strange metal states. A phenomenological theory which aims to describe the pseudo gap phase as one consisting of preformed bond-pairs, is required to include both unpaired electrons and Cooper pairs of the same electrons coexisting and necessarily coupled with each other. In our Ginzburg Landau approach only the latter are explicit, while the former are integrated out. However, effects connected with the pair degrees of freedom are often investigated via their coupling to electrons, one very prominent examples being Angle Resolved Photoemmision Spectroscopy(ARPES),in which the momentum and energy spectrum of electrons ejected from the metal impinged by photons is investigated. In Chapter 6, we develop a unified theory of electronic excitations in the superconducting and pseudo gap phases using a model of electrons quantum mechanically coupled to spatially and temporally fluctuating Cooper pairs(the nearest neighbour singlet bond pairs). We discuss the theory and a number of its predictions which seem to be in good agreement with high resolution ARPES measurements, which have uncovered a number of unusual spectral properties of electrons near the Fermi energy with definite in-plane momenta. We show here that the spectral function of electrons with momentum ranging over the putative Fermi surface(recovered at high temperatures above the pseudogap temperature scale) is strongly affected by their coupling to Cooper pairs. On approaching Tc i.e. the temperature at which the Cooper pair phase stiffness becomes nonzero, the inevitable coupling of electrons with long-wavelength(d-wave symmetry) phase fluctuations leads to the observed characteristic low-energy behavior as reported in Chapter 6. Collective d-wave symmetry superconducting correlations develop among the pairs with a characteristic correlation length ξ which diverges on approaching the continuous transition temperature Tc from above. These correlations have a generic form for distances much larger than the lattice spacing. As we show here, the effect of these correlations on the electrons leads, for example, to a pseudogap in electronic density of states for T > T c persisting till T* , temperature-dependent Fermi arcs i.e. regions on the Fermi surface where the quasiparticle spectral density is non zero for a zero energy excitation and to the filling of the antinodal pseudogap in the manner observed. Further, the observed long-range order(LRO) below c leads to a sharp antinodal spectral feature related to the non zero superfluid density, and thermal pair fluctuations cause a deviation(‘bending’) of the inferred ‘gap’ as a function of k from the expected d-wave form (cos kxa - cos kya). The bending, being of thermal origin, decreases with decreasing temperature, in agreement with recent ARPES measurements. I conclude in Chapter 7 by mentioning some natural directions in which the functional and the approach used here could be taken forward. The phenomenological theory proposed and developed in this thesis reconciles and ties together a range of cuprate superconductivity phenomena qualitatively and confronts them quantitatively with experiment. The results, and their agreement with a large body of experimental findings, strongly support the mechanism based on nearest neighbor Cooper pairs, and emergence of long-range -wave symmetry order as a collective effect arising from short range interaction between these pairs. This probably points to the way in which high-c superconductivity will be understood.

<p>This thesis is focused on studies of substituted Hg-based superconducting copper oxides ((Hg_1-x<i>M</i>_x)Ba₂Ca_n-1Cu_nO2_n+2+δ). These compounds are promising objects of investigation, not only from a fundamental point of view but also because of their high values of superconducting transition temperature (<i>T</i>_c) and irreversibility field (<i>H</i>_irr).</p><p>The first part of the thesis is devoted to optimization of the synthesis procedure for Hg-based cuprates. The influence of different parameters (<i>T</i>,<i> t</i>, <i>p</i>(Hg),<i> p</i>(O₂)) on the synthesis of these compounds in sealed silica tubes was studied. Optimal conditions yielded samples containing up to 95% of HgBa₂Ca₂Cu₃O_8+δ (Hg-1223). The formation of solid solutions with the formula (Hg_1-xCu_x)Ba₂Ca₂Cu₃O_8+δ (where x <= 0.5) was also established. Another technique was developed, using LiF as a flux, for synthesis of samples containing up to 90% of the HgBa₂CaCu₂O_6+δ (Hg-1212) phase.</p><p>The second part concerns synthesis and studies of oxyfluorides using Hg-1212 and Hg-1223 as starting materials together with XeF₂ as a fluorinating agent. It was found that oxyfluorides of both phases have a parabolic dependence of T_c vs. <i>a</i> parameter as well as enhanced <i>T</i>_c values (Δ<i>T</i> ≈ 3-4 K) in comparison with optimally doped non-fluorinated analogues. The crystal structure of Hg-1223 oxyfluoride was studied by X-ray powder and neutron diffraction methods. It is suggested that chemical modification of the crystal structure leads to a decrease in Cu-O distance without noticeable change in Cu-O-Cu angle (in the (CuO₂) layers), which may be the significant factors influencing this <i>T</i>_c increase. Hg-1223 oxyfluoride was also studied under high pressure for first time. It was found that this compound has a record-high <i>T</i>_c value (≈ 166 K) at <i>P</i> ≈ 23 GPa.</p><p>The last part describes the investigation of substituted Hg-based superconductors in the series (Hg_0.9M_0.1)Ba₂CuO_4+δ {(Hg,<i>M</i>)-1201}, where <i>M</i> = Tl, Pb, W, Mo, Nb and V. A comprehensive study of these compounds by various methods (X-ray powder diffraction, EDX, IR-, EXAFS- and XANES -spectroscopy) indicated that the change of charge carrier doping level is a crucial factor determining the irreversibility line. (Hg_0.9Mo_0.1)Ba₂CuO_4+δ showed the most improved irreversibility line position among the (Hg,<i>M</i>)-1201 compounds studied in this series.</p>

This thesis is focused on studies of substituted Hg-based superconducting copper oxides ((Hg1-xMx)Ba2Can-1CunO2n+2+δ). These compounds are promising objects of investigation, not only from a fundamental point of view but also because of their high values of superconducting transition temperature (Tc) and irreversibility field (Hirr). The first part of the thesis is devoted to optimization of the synthesis procedure for Hg-based cuprates. The influence of different parameters (T, t, p(Hg), p(O2)) on the synthesis of these compounds in sealed silica tubes was studied. Optimal conditions yielded samples containing up to 95% of HgBa2Ca2Cu3O8+δ (Hg-1223). The formation of solid solutions with the formula (Hg1-xCux)Ba2Ca2Cu3O8+δ (where x &lt;= 0.5) was also established. Another technique was developed, using LiF as a flux, for synthesis of samples containing up to 90% of the HgBa2CaCu2O6+δ (Hg-1212) phase. The second part concerns synthesis and studies of oxyfluorides using Hg-1212 and Hg-1223 as starting materials together with XeF2 as a fluorinating agent. It was found that oxyfluorides of both phases have a parabolic dependence of Tc vs. a parameter as well as enhanced Tc values (ΔT ≈ 3-4 K) in comparison with optimally doped non-fluorinated analogues. The crystal structure of Hg-1223 oxyfluoride was studied by X-ray powder and neutron diffraction methods. It is suggested that chemical modification of the crystal structure leads to a decrease in Cu-O distance without noticeable change in Cu-O-Cu angle (in the (CuO2) layers), which may be the significant factors influencing this Tc increase. Hg-1223 oxyfluoride was also studied under high pressure for first time. It was found that this compound has a record-high Tc value (≈ 166 K) at P ≈ 23 GPa. The last part describes the investigation of substituted Hg-based superconductors in the series (Hg0.9M0.1)Ba2CuO4+δ {(Hg,M)-1201}, where M = Tl, Pb, W, Mo, Nb and V. A comprehensive study of these compounds by various methods (X-ray powder diffraction, EDX, IR-, EXAFS- and XANES -spectroscopy) indicated that the change of charge carrier doping level is a crucial factor determining the irreversibility line. (Hg0.9Mo0.1)Ba2CuO4+δ showed the most improved irreversibility line position among the (Hg,M)-1201 compounds studied in this series.

Over the past twenty-five years, condensed matter physics has been developing materials with novel electronic characteristics for a wide range of future applications. Two research directions have shown particular promise: topological insulators, and high temperature copper based superconductors (cuprates). Topological insulators are a newly discovered class of materials that can be manipulated for spintronic or quantum computing devices. However there is a poor spectroscopic understanding of the current topological insulators and emerging topological insulator candidates. In cuprate superconductors, the challenge lies in raising the superconducting transition temperature to temperatures accessible in non-laboratory settings. This effort has been hampered by a poor understanding of the superconducting mechanism and its relationship with a mysterious pseudogap phase. In this thesis, I will describe experiments conducted on topological insulators and cuprate superconductors using scanning tunneling microscopy and spectroscopy, which provide nanoscale spectroscopic information in these materials. / Physics

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