A recent discovery of the pair density wave (PDW) order creates a stir in understanding an underlying physics in the pseudogap states of the cuprate high temperature superconductors. We have performed a Spectroscopic Imaging Scanning Tunneling Microscopy (SI-STM) measurements on Bi$_2$Sr$_2$CaCu$_2$O$_8$+$δ$ and identified that spatially uniform d-wave superconductivity (DSC), d-symmetry charge density wave (CDW), and the PDW play important roles in an intertwined fashion. In this review, we show how these different electronic degrees of freedom emerges in electronic structures of the cuprate and discuss how they are related to each other.
We report on atomic-scale visualization of the structure of infinite-layer cuprate SrCuO2 thin films grown on Nb-doped SrTiO3 substrates by molecular beam epitaxy. In-situ scanning tunneling microscopy study reveals stoichiometric copper oxide (CuO2) plane with a 2 x 2 surface reconstruction, prompted by preferential clustering of four adjacent CuO2 plaquettes. By imaging the subsurface Sr atoms, intra-unit-cell rotational symmetry breaking is observed, which, together with the adjacent CuO2 clustering, can be well accounted for by a periodic up-down buckling of oxygen ions on the CuO2 plane. …
We report magnetic optical second-harmonic generation (SHG) polarimetry and imaging on Sr$_2$Cu$_3$O$_4$Cl$_2$, which allows direct visualization of the mesoscopic antiferromagnetic (AFM) structure of a parent cuprate. Temperature- and magnetic-field-dependent SHG reveals large domains with 90$^{\circ}$ relative orientations that are stabilized by a combination of uniaxial magnetic anisotropy and the Earth's magnetic field. Below a temperature $T_R$ $\sim$ 97 K, we observe an unusual 90$^{\circ}$ spin reorientation transition, possibly driven by competing magnetic anisotropies of the two coppe…
Identifying the essence of doped Mott insulators is one of the major outstanding problems in condensed matter physics and the key to understanding the high-temperature superconductivity in cuprates. We report real space visualization of Mott transition in Sr1-xLaxCuO2+y cuprate films that cover the entire electron- and hole-doped regimes. Tunneling conductance measurements directly on the cooper-oxide (CuO2) planes reveal a systematic shift in the Fermi level, while the fundamental Mott-Hubbard band structure remains unchanged. This is further demonstrated by exploring atomic-scale electronic …
We investigate the low energy acoustical and optical modes in $\mathrm{HgBa_2CuO_{4+δ}}$ using inelastic x-ray scattering (IXS). The experimental phonon dispersion and the dynamical structure factor are compared with an atomic shell model, and the set of the atomic potentials obtained are discussed. Our results are also compared with those obtained by Raman spectroscopy and with density-of-state data measured by inelastic neutron scattering.
Many theoretical models of high temperature superconductivity focus only on the doping dependence of the CuO2 plane electronic structure. But such models are manifestly insufficient to explain the strong variations in superconducting critical temperature Tc among cuprates which have identical hole-density but are crystallographically different outside the CuO2 plane. A key challenge, therefore, has been to identify a predominant out-of-plane influence controlling the superconductivity - with much attention focusing on the distance $d_A$ between the apical oxygen and the planar copper atom. Her…
High temperature superconductivity in cuprates arises from doping a parent Mott insulator by electrons or holes. A central issue is how the Mott gap evolves and the low-energy states emerge with doping. Here we report angle-resolved photoemission spectroscopy measurements on a cuprate parent compound by sequential in situ electron doping. The chemical potential jumps to the bottom of the upper Hubbard band upon a slight electron doping, making it possible to directly visualize the charge transfer band and the full Mott gap region. With increasing doping, the Mott gap rapidly collapses due to t…
We suggest a model for electronic structure of cuprate superconductors that makes it possible to describe evolution of this structure with the doping and provides a new explanation for a number of typical features of cuprates, including the pseudogap and the Fermi arcs. According to this model, the unique electronic structure of cuprates is favorable for the formation of two-atomic negative-U centers (NUCs) and realization of a peculiar mechanism of the electron-electron interaction.
A major remaining challenge in the superconducting cuprates is the unambiguous differentiation of the composition and electronic structure of the CuO$_2$ layers and those of the intermediate layers. The large c axis for these materials permits employing soft x-ray (930.3 eV) standing wave (SW) excitation in photoemission that yields atomic layer-by-atomic layer depth resolution of these properties. Applying SW photoemission to Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ yields the depth distribution of atomic composition and the layer-resolved densities of states. We detect significant Ca presence in the Sr…
The defining characteristic of hole-doped cuprates is $d$-wave high temperature superconductivity. However, intense theoretical interest is now focused on whether a pair density wave state (PDW) could coexist with cuprate superconductivity (D. F. Agterberg et al., Annual Review of Condensed Matter Physics 11, 231 (2020)). Here, we use a strong-coupling mean-field theory of cuprates, to model the atomic-scale electronic structure of an eight-unit-cell periodic, $d$-symmetry form factor, pair density wave (PDW) state coexisting with $d$-wave superconductivity (DSC). From this PDW+DSC model, the …
Although the mechanism of superconductivity in the cuprates remains elusive, it is generally agreed that at the heart of the problem is the physics of doped Mott insulators. The cuprate parent compound has one unpaired electron per Cu site, and is predicted by band theory to be a half-filled metal. The strong onsite Coulomb repulsion, however, prohibits electron hopping between neighboring sites and leads to a Mott insulator ground state with antiferromagnetic (AF) ordering. Charge carriers doped into the CuO2 plane destroy the insulating phase and superconductivity emerges as the carrier dens…
The identity of the fundamental broken symmetry (if any) in the underdoped cuprates is unresolved. However, evidence has been accumulating that this state may be an unconventional density wave. Here we carry out site-specific measurements within each CuO$_2$ unit-cell, segregating the results into three separate electronic structure images containing only the Cu sites (Cu(r)) and only the x/y-axis O sites (O$_x$(r) and O$_y$(r)). Phase resolved Fourier analysis reveals directly that the modulations in the O$_x$(r) and O$_y$(r) sublattice images consistently exhibit a relative phase of $π$. We …
We use scanning tunneling microscopy to visualize the atomic-scale electronic states induced by a pair of hole dopants in Ca2CuO2Cl2 parent Mott insulator of cuprates. We find that when the two dopants approach each other, the transfer of spectral weight from high energy Hubbard band to low energy in-gap state creates a broad peak and nearly V-shaped gap around the Fermi level. The peak position shows a sudden drop at distance around 4 a0 and then remains almost constant. The in-gap states exhibit peculiar spatial distributions depending on the configuration of the two dopants relative to the …
We propose a simple method of calculating inhomogeneous, atomic-scale phenomena in superconductors which makes use of the wave function information traditionally discarded in the construction of tight-binding models used in the Bogoliubov-de Gennes equations. The method uses symmetry based first principles Wannier functions to visualize the effects of superconducting pairing on the distribution of electronic states over atoms within a crystal unit cell. Local symmetries lower than the global lattice symmetry can thus be exhibited as well, rendering theoretical comparisons with scanning tunneli…
Theories based upon strong real space (r-space) electron electron interactions have long predicted that unidirectional charge density modulations (CDM) with four unit cell (4$a_0$) periodicity should occur in the hole doped cuprate Mott insulator (MI). Experimentally, however, increasing the hole density p is reported to cause the conventionally defined wavevector $Q_A$ of the CDM to evolve continuously as if driven primarily by momentum space (k-space) effects. Here we introduce phase resolved electronic structure visualization for determination of the cuprate CDM wavevector. Remarkably, this…
Recent scanning tunneling spectroscopy experiments have provided evidence that dopant impurities in high- Tc superconductors can strongly modify the electronic structure of the CuO2 planes nearby, and possibly influence the pairing. To investigate this connection, we calculate the local magnetic superexchange J between Cu ions in the presence of dopants within the framework of the three-band Hubbard model, up to fifth-order in perturbation theory. We demonstrate that the sign of the change in J depends on the relative dopant-induced spatial variation of the atomic levels in the CuO2 plane, con…
We present a microscopic derivation of the nematic charge-density-wave (CDW) formation in cuprate superconductors based on the three-orbital d-p Hubbard model, by introducing the vertex correction (VC) into the charge susceptibility. The CDW instability at $q=(Δ_{FS},0)$, $(0,Δ_{FS})$ appears when the spin fluctuations are strong, due to the strong charge-spin interference represented by the VC. Here, $Δ_{FS}$ is the wavenumber between the neighboring hot spots. The obtained spin-fluctuation-driven CDW is expressed as the "intra-unit-cell orbital order" accompanied by the charge transfer betwe…
The most intriguing observation of cuprate experiments is most likely the metal-insulator-crossover (MIC), seen in the underdome region of the temperature-doping phase diagram of copper-oxides under a strong magnetic field, when the superconductivity is suppressed. This MIC, which results in such phenomena as heat conductivity downturn, anomalous Lorentz ratio, nonlinear entropy, insulating ground state, nematicity- and stripe-phases and Fermi pockets, reveals the nonconventional dielectric property of the pseudogap-normal phase. Since conventional superconductivity appears from a conducting n…
A detailed Linear Combination of Atomic Orbitals (LCAO) tight-binding model is developed for the layered High-Temperature Superconductor cuprates. The band structure of these materials is described using a sigma-band Hamiltonian employing Cu4s, Cu3d_x^2-y^2, O2p_x and O2p_y atomic orbitals. The Fermi level and the shape of the resulting Fermi surface are fitted to recent Angle Resolved Photon Emission Spectroscopy (ARPES) data to realistically determine the dispersion in the conduction band. Electron-electron interactions and, ultimately, Cooper pairing is obtained by introducing a Heitler-Lon…
Removing electrons from the CuO2 plane of cuprates alters the electronic correlations sufficiently to produce high-temperature superconductivity. Associated with these changes are spectral weight transfers from the high energy states of the insulator to low energies. In theory, these should be detectable as an imbalance between the tunneling rate for electron injection and extraction - a tunneling asymmetry. We introduce atomic-resolution tunneling-asymmetry imaging, finding virtually identical phenomena in two lightly hole-doped cuprates: Ca1.88Na0.12CuO2Cl2 and Bi2Sr2Dy0.2Ca0.8Cu2O8+d. Inten…
Extensive research into high temperature superconducting cuprates is now focused upon identifying the relationship between the classic 'pseudogap' phenomenon$^{1,2}$ and the more recently investigated density wave state$^{3-13}$. This state always exhibits wave vector $Q$ parallel to the planar Cu-O-Cu bonds$^{4-13}$ along with a predominantly $d$-symmetry form factor$^{14-17}$ (dFF-DW). Finding its microscopic mechanism has now become a key objective$^{18-30}$ of this field. To accomplish this, one must identify the momentum-space ($k$-space) states contributing to the dFF-DW spectral weight,…
The most essential characteristic of any fluid is the velocity field v(r) and this is particularly true for macroscopic quantum fluids. Although rapid advances have occurred in quantum fluid v(r) imaging, the velocity field of a charged superfluid - a superconductor - has never been visualized. Here we use superconductive-tip scanning tunneling microscopy to image the electron-pair density \r{ho}_S(r) and velocity v_S(r) fields of the flowing electron-pair fluid in superconducting NbSe2. Imaging v_S(r) surrounding a quantized vortex finds speeds reaching 10,000 km/hr. Together with independent…
In complex transition metal oxide heterostructures of physically dissimilar perovskite compounds, interface phenomena can lead to novel physical properties not observed in either of their constituents. This remarkable feature opens new prospects for technological applications in oxide electronic devices based on nm-thin oxide films. Here we report on a significant electronic charge and orbital reconstruction at interfaces between YBa2Cu3O6 and SrTiO3 studied using local spin density approximation (LSDA) with intra-atomic Coulomb repulsion (LSDA+U). We show that the interface polarity results i…
In this paper we present an overview of radio frequency (RF) spectroscopy in the atomic Fermi superfluids. An ultimate goal is to suggest new directions in the cold gas research agenda from the condensed matter perspective.Our focus is on the experimental and theoretical literature of cold gases and photoemission spectroscopy of the cuprates particularly as it pertains to areas of overlap. This paper contains a systematic overview of the theory of RF spectroscopy, both momentum integrated and momentum resolved. We discuss the effects of traps, population imbalance, final state interactions ove…
Cuprates are promising candidates for study in developing higher temperature superconductors. A thorough understanding of a material's phonon modes enables further investigation of its emergent properties, however, no complete reference of the phonon modes exists. Here, using density functional theory, we evaluate the phonon frequencies and atomic displacements for $\text{La}_2\text{CuO}_4$, $\text{Bi}_2\text{Sr}_2\text{CuO}_6$, and $\text{Bi}_2\text{Sr}_2\text{CaCu}_2\text{O}_8$ in their tetragonal structures. The phonon modes for all materials agree with those expected from space group symme…
There is a growing compelling experimental evidence that a quantum complex matter scenario made of multiple electronic components, and competing quantum phases is needed to grab the key physics of high critical temperature (Tc) superconductivity in layered cuprates. While it is known that defects self-organization controls Tc, the mechanism remains an open issue. Here we focus on the theoretical prediction of the multi-band electronic structure and the formation of broken Fermi surfaces generated by the self-organization of oxygen interstitials O-i atomic wires in the spacer layers in HgBa2CuO…
Recent low-temperature scanning tunnelling spectroscopy experiments on the surface of BSCCO-2212 have revealed a strong positive correlation between the position of localized resonances at -960 meV identified with interstitial oxygen dopants and the size of the local spectral gap. We review efforts to understand these correlations within a model where the dopants modulate the pair interaction on an atomic scale. We provide further evidence for this model by comparing the correlations between the dopants and the local density of states with experimental results.
The concept of stimulated emission of bosons has played an important role in modern science and technology, and constitutes the working principle for lasers. In a stimulated emission process, an incoming photon enhances the probability that an excited atomic state will transition to a lower energy state and generate a second photon of the same energy. It is expected, but not experimentally shown, that stimulated emission contributes significantly to the zero resistance current in a superconductor by enhancing the probability that scattered Cooper pairs will return to the macroscopically occupi…
The $d$-$wave$ superconductivity is analyzed within the three-band $d$-$p$ model with the use of the diagrammatic expansion of the Guztwiller wave function method (DE-GWF). The determined stability regime of the superconducting state appears in the range of hole doping $δ\lesssim 0.35$, with the optimal doping close to $δ\approx 0.19$. The pairing amplitudes between the $d$-orbitals due to copper and $p_x/p_y$ orbitals due to oxygen are analyzed together with the hybrid $d$-$p$ pairing. The $d$-$d$ pairing between the nearest neighboring atomic sites leads to the dominant contribution to the S…
One of the key motivations for the development of atomically resolved spectroscopic imaging STM (SI-STM) has been to probe the electronic structure of cuprate high temperature superconductors. In both the d-wave superconducting (dSC) and the pseudogap (PG) phases of underdoped cuprates, two distinct classes of electronic states are observed using SI-STM. The first class consists of the dispersive Bogoliubov quasiparticles of a homogeneous d-wave superconductor. These are detected below a lower energy scale |E|=Δ0 and only upon a momentum space (k-space) arc which terminates near the lines conn…
We introduce and study an XY-type model of thermal and quantum phase fluctuations in a two-dimensional correlated lattice d-wave superconductor based on the QED3 effective theory of high temperature superconductors. General features of and selected results obtained within this model were reported earlier in an abbreviated format (Z. Tesanovic, cond-mat/0405235). The model is geared toward describing not only the long distance but also the intermediate lengthscale physics of underdoped cuprates. In particular, we elucidate the dynamical origin and investigate specific features of the Cooper pai…
X-ray techniques have been used for more than a century to study the atomic and electronic structure in virtually any type of material. The advent of correlated electron systems, in particular complex oxides, brought about new scientific challenges and opportunities for the advancement of conventional x-ray methods. In this context, the need for new approaches capable of selectively sensing new forms of orders involving all degrees of freedom -- charge, orbital, spin, and lattice -- paved the way for the emergence and success of resonant x-ray scattering, which has become an increasingly popul…
Due to nontrivial orbital pairing symmetry, surfaces and interfaces of high-Tc superconductors sup- port states which violate time-reversal (T -) symmetry. Such naturally degenerate states, useful as work- ing states of a qubit, are standard for atomic or molecular-size qubit prototypes (e.g. based on nuclear spins), but exceptional for mesoscopic qubits. (In particular, they hold promise of a better scalability.) In these lectures I review the physics of T -breaking on surfaces and interfaces of high-Tc superconductors; then describe existing proposals for high-Tc based qubits and the current…
A consistent microscopic theory of pseudogap phenomena and novel Bose-liquid superconductivity (superfluidity) is presented, based on the fact that in high-$T_c$ cuprates and related systems the energy $\varepsilon_A$ of the effective attraction between fermions is comparable with their Fermi energy $\varepsilon_F$ and the bosonic Cooper pairs are formed above $T_c$ and then a part of such Cooper pairs condense into a Bose superfluid at $T_c$. High-$T_c$ cuprates and other systems with low Fermi energies ($\varepsilon_F\sim\varepsilon_A$) are bosonic superconductors/superfluids and exhibit pse…
High temperature superconductivity emerges in unique materials, like cuprates, that belong to the class of heterostructures at atomic limit, made of a superlattice of superconducting atomic layers intercalated by spacer layers. The physical properties of a strongly correlated electronic system, emerge from the competition between different phases with a resulting inhomogeneity from nanoscale to micron scale. Here we focus on the spatial arrangements of two types of structural defects in the cuprate La2CuO4+y : i) the local lattice distortions in the CuO2 active layers and ii) the lattice disto…
Recent progress in two-dimensional superconductors with atomic-scale thicknesses is reviewed mainly from the experimental point of view. The superconducting systems treated here involve a variety of materials and forms: elemental-metal ultrathin films and atomic layers on semiconductor surfaces; interfaces and superlattices of heterostructures made of cuprates, perovskite oxides, and rare-earth metal heavy-fermion compounds; interfaces of electric-double-layer transistors; graphene and atomic sheets of transition-metal dichalcogenide; iron selenide and organic conductors on oxide and metal sur…
The local electronic structures of La2CuO4, three members of the Yttrium-family (YBa2Cu3O6, YBa2Cu3O7, and YBa2Cu4O8), and to some extent of Nd2CuO4 have been determined using all-electron ab-initio cluster calculations for clusters comprising up to thirteen planar copper atoms associated with their nearest planar and apical oxygen atoms. Spin-polarized calculations in the framework of density functional theory have enabled an estimation of the superexchange couplings J. Electric field gradients at the planar copper sites are determined and their dependence on the occupation of the various ato…
We use scanning tunneling microscopy (STM) to study magnetic Fe impurities intentionally doped into the high-temperature superconductor Bi$_{2}$Sr$_{2}$Ca$_{2}$CuO$_{8+δ}$. Our spectroscopic measurements reveal that Fe impurities introduce low-lying resonances in the density of states at Ω$_{1}$ $\approx$ 4meV and Ω$_{2}$ $\approx$ 15 meV allowing us to determine that, despite having a large magnetic moment, potential scattering of quasiparticles by Fe impurities dominates magnetic scattering. In addition, using high-resolution spatial characterizations of the local density of states near and …
The criteria for bosonization of Cooper pairs and novel Bose-liquid superconductivity and superfluidity in high-$T_c$ cuprates and other pseudogap matters are formulated by using the uncertainty principle and the boson mean field theory. We argue that the BCS-type s- or d-wave superconductivity occurring in the fermionic limit of Cooper pairs (which exist in ordinary metals and heavily overdoped cuprates with large Fermi energies) is not characteristic of underdoped to overdoped cuprates with low Fermi energies. The superconducting order parameter in high-$T_c$ cuprates and other pseudogap mat…
Since the discovery of high temperature superconductivity in cuprates, Josephson junction based phase-sensitive experiments are believed and used to provide the most convincing evidence for determining the pairing symmetry. Regardless of different junction materials and geometries used, quantum tunneling involved in these experiments is essentially a nanoscale process, and thus, actual experimental results are extremely sensitive to atomic details of the junction structures. The situation has led to controversial results as to the nature of the pairing symmetry of cuprates: while in-plane junc…
We study a toy model for a superconductor on a bipartite lattice, where intrinsic pairing inhomogeneity is produced by two different coupling constants on the sublattices. The simplicity of the model allows for analytic solutions and tests of the consequences of atomic-scale variations in pairing interactions which have been considered recently in the cuprates. We present results for the transition temperature, density of states, and thermodynamics of the system over a phase diagram in the plane of two pairing coupling constants. For coupling constants of alternating sign, a gapless supercondu…
