Comparing first-principles density functionals plus corrections for the lattice dynamics of YBa2Cu3O6.

The enigmatic mechanism underlying unconventional high-temperature superconductivity, especially the role of lattice dynamics, has remained a subject of debate. Theoretical insights have long been hindered due to the lack of an accurate first-principles description of the lattice dynamics of cuprates. Recently, using the r2SCAN meta-generalized gradient approximation (meta-GGA) functional, we have been able to achieve accurate phonon spectra of an insulating cuprate YBa2Cu3O6 and discover significant magnetoelastic coupling in experimentally interesting Cu-O bond stretching optical modes [Ning et al., Phys. Rev. B 107, 045126 (2023)]. We extend this work by comparing Perdew-Burke-Ernzerhof and r2SCAN performances with corrections from the on-site Hubbard U and the D4 van der Waals (vdW) methods, aiming at further understanding on both the materials science side and the density functional side. We demonstrate the importance of vdW and self-interaction corrections for accurate first-principles YBa2Cu3O6 lattice dynamics. Since r2SCAN by itself partially accounts for these effects, the good performance of r2SCAN is now more fully explained. In addition, the performances of the Tao-Mo series of meta-GGAs, which are constructed in a different way from the strongly constrained and appropriately normed (SCAN) meta-GGA and its revised version r2SCAN, are also compared and discussed.

Competing stripe and magnetic phases in the cuprates from first principles.

Realistic description of competing phases in complex quantum materials has proven extremely challenging. For example, much of the existing density-functional-theory-based first-principles framework fails in the cuprate superconductors. Various many-body approaches involve generic model Hamiltonians and do not account for the interplay between the spin, charge, and lattice degrees of freedom. Here, by deploying the recently constructed strongly constrained and appropriately normed (SCAN) density functional, we show how the landscape of competing stripe and magnetic phases can be addressed on a first-principles basis both in the parent insulator YBa2Cu3O6 and the near-optimally doped YBa2Cu3O7 as archetype cuprate compounds. In YBa2Cu3O7, we find many stripe phases that are nearly degenerate with the ground state and may give rise to the pseudogap state from which the high-temperature superconducting state emerges. We invoke no free parameters such as the Hubbard U, which has been the basis of much of the existing cuprate literature. Lattice degrees of freedom are found to be crucially important in stabilizing the various phases.

Nanoscale interplay of strain and doping in a high-temperature superconductor.

The highest-temperature superconductors are electronically inhomogeneous at the nanoscale, suggesting the existence of a local variable that could be harnessed to enhance the superconducting pairing. Here we report the relationship between local doping and local strain in the cuprate superconductor Bi(2)Sr(2)CaCu(2)O(8+x). We use scanning tunneling microscopy to discover that the crucial oxygen dopants are periodically distributed in correlation with local strain. Our picoscale investigation of the intraunit-cell positions of all oxygen dopants provides essential structural input for a complete microscopic theory.

Causal structure of interacting Weyl fermions in condensed matter systems.

The spacetime light cone is central to the definition of causality in the theory of relativity. Recently, links between relativistic and condensed matter physics have been uncovered, where relativistic particles can emerge as quasiparticles in the energy-momentum space of matter. Here, we unveil an energy-momentum analogue of the spacetime light cone by mapping time to energy, space to momentum, and the light cone to the Weyl cone. We show that two Weyl quasiparticles can only interact to open a global energy gap if they lie in each other's energy-momentum dispersion cones-analogous to two events that can only have a causal connection if they lie in each other's light cones. Moreover, we demonstrate that the causality of surface chiral modes in quantum matter is entangled with the causality of bulk Weyl fermions. Furthermore, we identify a unique quantum horizon region and an associated 'thick horizon' in the emergent causal structure.

Topological Antiferromagnetic Van der Waals Phase in Topological Insulator/Ferromagnet Heterostructures Synthesized by a CMOS-Compatible Sputtering Technique.

Breaking time-reversal symmetry by introducing magnetic order, thereby opening a gap in the topological surface state bands, is essential for realizing useful topological properties such as the quantum anomalous Hall and axion insulator states. In this work, a novel topological antiferromagnetic (AFM) phase is created at the interface of a sputtered, c-axis-oriented, topological insulator/ferromagnet heterostructure-Bi2 Te3 /Ni80 Fe20 because of diffusion of Ni in Bi2 Te3 (Ni-Bi2 Te3 ). The AFM property of the Ni-Bi2 Te3 interfacial layer is established by observation of spontaneous exchange bias in the magnetic hysteresis loop and compensated moments in the depth profile of the magnetization using polarized neutron reflectometry. Analysis of the structural and chemical properties of the Ni-Bi2 Te3 layer is carried out using selected-area electron diffraction, electron energy loss spectroscopy, and X-ray photoelectron spectroscopy. These studies, in parallel with first-principles calculations, indicate a solid-state chemical reaction that leads to the formation of Ni-Te bonds and the presence of topological antiferromagnetic (AFM) compound NiBi2 Te4 in the Ni-Bi2 Te3 interface layer. The Neél temperature of the Ni-Bi2 Te3 layer is ≈63 K, which is higher than that of typical magnetic topological insulators (MTIs). The presented results provide a pathway toward industrial complementary metal-oxide-semiconductor (CMOS)-process-compatible sputtered-MTI heterostructures, leading to novel materials for topological quantum devices.

Understanding the magnetic interaction between intrinsic defects and impurity ions in room-temperature ferromagnetic Mg1-xFexO thin films.

Understanding the nature and characteristics of the intrinsic defects and impurities in the dielectric barrier separating the ferromagnetic electrodes in a magnetic tunneling junction is of great importance for understanding the often observed 'barrier-breakdown' therein. In this connection, we present herein systematic experimental (SQUID and synchrotron-radiation-based x-ray absorption spectroscopy) and computational studies on the electronic and magnetic properties of Mg1-xFexO thin films. Our studies reveal: (i) defect aggregates comprised of basic and trimer units (Fe impurity coupled to 1 or 2 Mg vacancies) and (ii) existence of two competing magnetic orders, defect- and dopant-induced, with spin densities aligning anti-parallel if the trimer is present in the oxide matrix. These findings open up new avenues for designing tunneling barriers with high endurance and tunneling effect upon tuning the concentration/distribution of the two magnetic orders.

Fermi-surface-free superconductivity in underdoped (Bi,Pb)(Sr,La)2CuO(6+δ) (Bi2201).

Fermi-surface-free superconductivity arises when the superconducting order pulls down spectral weight from a band that is completely above the Fermi energy in the normal state. We show that this can arise in hole-doped cuprates when a competing order causes a reconstruction of the Fermi surface. The change in Fermi surface topology is accompanied by a characteristic rise in the spectral weight. Our results support the presence of a trisected superconducting dome, and suggest that superconductivity is responsible for stabilizing the (π,π) magnetic order at higher doping.

The changing colors of a quantum-confined topological insulator.

Bismuth selenide (Bi2Se3) is a 3D topological insulator, its strong spin-orbit coupling resulting in the well-known topologically protected coexistence of gapless metallic surface states and semiconducting bulk states with a band gap, Eg ≃ 300 meV. A fundamental question of considerable importance is how the electronic properties of this material evolve under nanoscale confinement. We report on catalyst-free, high-quality single-crystalline Bi2Se3 with controlled lateral sizes and layer thicknesses that could be tailored down to a few nanometers and a few quintuple layers (QLs), respectively. Energy-resolved photoabsorption spectroscopy (1.5 eV < E(photon) < 6 eV) of these samples reveals a dramatic evolution of the photon absorption spectra as a function of size, transitioning from a featureless metal-like spectrum in the bulk (corresponding to a visually gray color), to one with a remarkably large band gap (Eg ≥ 2.5 eV) and a spectral shape that correspond to orange-red colorations in the smallest samples, similar to those seen in semiconductor nanostructures. We analyze this colorful transition using ab initio density functional theory and tight-binding calculations which corroborate our experimental findings and further suggest that while purely 2D sheets of few QL-thick Bi2Se3 do exhibit small band gaps that are consistent with previous ARPES results, the presently observed large gaps of a few electronvolts can only result from a combined effect of confinement in all three directions.

Fermi surface and pseudogap evolution in a cuprate superconductor.

The unclear relationship between cuprate superconductivity and the pseudogap state remains an impediment to understanding the high transition temperature (T(c)) superconducting mechanism. Here, we used magnetic field-dependent scanning tunneling microscopy to provide phase-sensitive proof that d-wave superconductivity coexists with the pseudogap on the antinodal Fermi surface of an overdoped cuprate. Furthermore, by tracking the hole-doping (p) dependence of the quasi-particle interference pattern within a single bismuth-based cuprate family, we observed a Fermi surface reconstruction slightly below optimal doping, indicating a zero-field quantum phase transition in notable proximity to the maximum superconducting T(c). Surprisingly, this major reorganization of the system's underlying electronic structure has no effect on the smoothly evolving pseudogap.

Imaging the impact of single oxygen atoms on superconducting Bi(2+y)Sr(2-y)CaCu2O(8+x).

High-temperature cuprate superconductors display unexpected nanoscale inhomogeneity in essential properties such as pseudogap energy, Fermi surface, and even superconducting critical temperature. Theoretical explanations for this inhomogeneity have ranged from chemical disorder to spontaneous electronic phase separation. We extend the energy range of scanning tunneling spectroscopy on Bi(2+y)Sr(2-y)CaCu(2)O(8+x), allowing a complete mapping of two types of interstitial oxygen dopants and vacancies at the apical oxygen site. We show that the nanoscale spatial variations in the pseudogap states are correlated with disorder in these dopant concentrations, particularly that of apical oxygen vacancies.