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All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Ab initio description of the Bi 2 Sr 2 CaCu 2 O 8+δ electronic structure

Bi-based cuprate superconductors are important materials for both fundamental research and applications. As in other cuprates, the superconducting phase in the Bi compounds lies close to an antiferromagnetic phase. Here, our density functional theory calculations based on the strongly-constrained-and-appropriately-normed exchange correlation functional in Bi 2 Sr 2 CaCu 2 O 8+δ reveal the persistence of magnetic moments on the copper ions for oxygen concentrations ranging from the pristine phase to the optimally hole-doped compound. We also find the existence of ferrimagnetic solutions in the heavily doped compounds, which are expected to suppress superconductivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Twofold symmetry of proximity-induced superconductivity in Bi 2 Te 3 / Bi 2 Sr 2 CaCu 2 O 8 + δ heterostructures revealed by scanning tunneling microscopy

We observe proximity-induced superconductivity in in situ prepared heterostructures constructed by topological insulator Bi 2 Te 3 thin films and high-temperature cuprate superconductors Bi 2 Sr 2 CaCu 2 O 8+δ . The superconducting gap maximum is about 7.6 meV on the surface of Bi 2 Te 3 thin films with a thickness of two quintuple layers, and the gap value decreases with an increase in the film thickness. Moreover, the quasiparticle interference data show clear evidence of a twofold symmetric superconducting gap with gap minima along one pair of the principal crystalline axes of Bi 2 Te 3 . This gap form is consistent with the Δ 4y notation of the topological superconductivity proposed in such systems. Our results provide fruitful information on the possible topological superconductivity induced by the proximity effect in high-temperature superconducting cuprates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Doping-dependent phonon anomaly and charge-order phenomena in the HgBa 2 CuO 4 + δ and HgBa 2 CaCu 2 O 6 + δ superconductors

Using resonant x-ray diffraction and Raman spectroscopy, we study charge correlations and lattice dynamics in two model cuprates, HgBa 2 CuO 4 + δ and HgBa 2 CaCu 2 O 6 + δ . We observe a maximum of the characteristic charge order temperature around the same hole concentration (p ≈ 0.09) in both compounds, and concomitant pronounced anomalies in the lattice dynamics that involve the motion of atoms in and/or adjacent to the CuO 2 layers. These anomalies are already present at room temperature, and therefore precede the formation of the static charge correlations, and we attribute them to an instability of the CuO 2 layers. Our finding implies that the charge order in the cuprates is an emergent phenomenon, driven by a fundamental variation in both lattice and electronic properties as a function of doping.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Extracting correlation effects from momentum-resolved electron energy loss spectroscopy: Synergistic origin of the dispersion kink in Bi 2.1 Sr 1.9 CaCu 2 O 8 + x

We employ momentum-resolved electron energy loss spectroscopy (M-EELS) on Bi 2.1 Sr 1.9 CaCu 2 O 8 + x to resolve the issue of the kink feature in the electron dispersion widely observed in the cuprates. To this end, we utilize the GW approximation to relate the density response function measured in M-EELS to the self-energy, isolating contributions from phonons, electrons, and the momentum dependence of the effective interaction to the decay rates. The phononic contributions, present in the M-EELS spectra due to electron-phonon coupling, lead to kink features in the corresponding single-particle spectra at energies between 40 and 80 meV, independent of the doping level. We find that a repulsive interaction constant in momentum space is able to yield the kink attributed to phonons in ARPES. Hence, our analysis of the M-EELS spectra points to local repulsive interactions as a factor that enhances the spectroscopic signatures of electron-phonon coupling in cuprates. We conclude that the strength of the kink feature in cuprates is determined by the combined action of electron-phonon coupling and electron-electron interactions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Universal relation between doping content and normal-state resistance in gate voltage tuned ultrathin Bi 2 Sr 2 CaCu 2 O 8 + x flakes

We report gate voltage tunable ultra-thin high-T c cuprates supply a unique platform to investigate the electronic phase diagram and superconductor-insulator transition. One of the challenges in this field is the precise determination of the doping content in the underdoped non-superconducting region. Here we report the discovery of a universal relation between the doping content p and the normal-state resistance at a fixed temperature R(T f ), p = α + β ln[1/R(T f )], in the ultra-thin Bi 2 Sr 2 CaCu 2 O 8+x flakes. The in-depth analysis shows that the evolution of carrier scattering probability with doping content and the change of effective mass caused by superconductor-insulator transition are two key factors leading to this logarithmic relation. Based on our finding, the more precise electronic phase diagram can be established. In addition, the superconductor-insulator transition is verified to be a quantum phase transition using a finite size scaling analysis. The scaling exponent z v is found to have a close correlation with the disorder levels. The present result provides an important foundation to investigate the fascinating electronic states in the ultra-thin cuprates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Persistent Josephson tunneling between Bi 2 Sr 2 CaCu 2 O 8 + x flakes twisted by 45 ° across the superconducting dome

There is a heated debate on the Josephson effect in twisted Bi 2 Sr 2 CaCu 2 O 8+x flakes. Recent experimental results suggest the presence of either anomalously isotropic pairing or exotic d+id-wave pairing, in addition to the commonly believed d-wave one. Here, we address this controversy by fabricating ultraclean junctions with uncompromised crystalline quality and stoichiometry at the junction interfaces. In the optimally doped regime, we obtain prominent Josephson coupling (2-4 mV) in multiple junctions with the twist angle of 45°, in sharp contrast to a recent report that shows two orders of magnitude suppression around 45° from the value at 0°. We further extend this study to the previously unexplored overdoped regime and observe pronounced Josephson tunneling at 45° together with Josephson diode effect up to 50 K. In conclusion, our work helps establish the persistent presence of an isotropic pairing component across the entire superconducting phase diagram.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Consistency between reflection momentum-resolved electron energy loss spectroscopy and optical spectroscopy measurements of the long-wavelength density response of Bi 2 Sr 2 CaCu 2 O 8 + x

The density fluctuation spectrum captures many fundamental properties of strange metals. Using momentum-resolved electron energy-loss spectroscopy (M-EELS), we recently showed that the density response of the strange metal Bi 2 Sr 2 CaCu 2 O 8+x (Bi-2212) at large momentum, q, exhibits a constant-in-frequency continuum reminiscent of the marginal Fermi liquid (MFL) hypothesis of the late 1980s. However, reconciling this observation with infrared (IR) optics experiments, which show a well-defined plasmon excitation at q ~ 0, has been challenging. Here we report M-EELS measurements of Bi-2212 using 4× improved momentum resolution, allowing us to reach the optical limit. For momenta q < 0.04 r.l.u., the M-EELS data show a plasmon feature that is quantitatively consistent with IR optics. For q > 0.04 r.l.u., the spectra become incoherent with an MFL-like, constant-in-frequency form. Here we speculate that, at finite frequency, ω, and nonzero q, some attribute of this Planckian metal randomizes the probe electron, causing it to lose information about its own momentum.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Shallow core levels, or how to determine the doping and T c of Bi 2 Sr 2 CaCu 2 O 8 + δ and Bi 2 Sr 2 CuO 6 + δ without cooling

In this study, determining the doping level in high-temperature cuprate superconductors is crucial for understanding the origin of superconductivity in these materials and for unlocking their full potential. However, accurately determining the doping level remains a significant challenge due to a complex interplay of factors and limitations in various measurement techniques. In particular, in Bi 2 Sr 2 CuO 6+δ and Bi 2 Sr 2 CaCu 2 O 8+δ , where the mobile carriers are introduced by non-stoichiometric oxygen δ, the determination has been extremely problematic. Here, we study the doping dependence of the electronic structure of these materials in angle-resolved photoemission and find that both the doping level, p, and the superconducting transition temeprature, T c can be precisely determined from the binding energy of the Bi 5d core-levels. The measurements can be performed at room temperature, enabling the determination of p and T c without cooling the samples. This should be very helpful for further studies of these materials

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Ultrafast Raman probe of the photoinduced superconducting to normal state transition in the cuprate Bi 2 ⁢Sr 2 ⁢CaCu 2 ⁢O 8+𝛿

Here, we report an ultrafast Time-Resolved Raman scattering study of the out-of-equilibrium photoinduced dynamics across the superconducting to normal state phase transition of the cuprate Bi 2 ⁢Sr 2⁢ CaCu 2 ⁢O 8+𝛿 . Using the polarization-resolved momentum space selectivity of Raman scattering, we track the superconducting condensate destruction and recovery dynamics with subpicoseconds time resolution in the antinodal region of the Fermi surface where the superconducting gap is maximum. Leveraging ultrafast Raman thermometry, we find a significant dichotomy between the superconducting condensate and the quasiparticle temperature dynamics near the antinodes, which cannot be framed in terms of a single effective electron temperature. The present work demonstrates the ability of Time-Resolved Raman scattering to selectively probe out-of-equilibrium pathways of different electronic subdegrees of freedom during a photoinduced phase transition.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Surface deposition of nanometer scale carbon structures on Bi 2 Sr 2 CaCu 2 O 8+δ using a low-cost scanning electron microscope

In this work, we investigate optically active nanostructures on Bi 2 Sr 2 CaCu 2 O 8+δ (BSCCO). The nanostructures are constructed from carbon nanocrystals formed using the electron beam of a scanning electron microscope to locally decompose residual hydrocarbons at the BSCCO surface. Atomic force microscopy is used to characterize the dimensions of these structures as a function of beam exposure time. This technique has been used to induce localized intercalation to form carbon nanoparticles up to tens of nanometers into a variety of 2D materials. Cross-sectional scanning transmission electron microscopy in BSCCO shows the presence of these carbon deposits on the surface, but there is no evidence they penetrate into the BSCCO substrate. Therefore, this technique is not suitable for localized intercalation in BSCCO, and it does have promise as a cost-effective approach to pattern nanometer scale etch stops.

2D materials↗
DOE OSTI2023

Low-energy quasi-circular electron correlations with charge order wavelength in Bi 2 Sr 2 CaCu 2 O 8+δ

Most resonant inelastic x-ray scattering (RIXS) studies of dynamic charge order correlations in the cuprates have focused on the high-symmetry directions of the copper oxide plane. However, scattering along other in-plane directions should not be ignored as it may help understand, for example, the origin of charge order correlations or the isotropic scattering resulting in strange metal behavior. Our RIXS experiments reveal dynamic charge correlations over the qx-qy scattering plane in underdoped Bi 2 Sr 2 CaCu 2 O 8+δ . Tracking the softening of the RIXS-measured bond-stretching phonon, we show that these dynamic correlations exist at energies below approximately 70 meV and are centered around a quasi-circular manifold in the q x -q y scattering plane with radius equal to the magnitude of the charge order wave vector, q CO . This phonon-tracking procedure also allows us to rule out fluctuations of short-range directional charge order (i.e., centered around [q x = ±q CO , q y = 0] and [q x = 0, q y = ±q CO ]) as the origin of the observed correlations.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Search for Q ~0 Order near a Forbidden Bragg Position in Bi 2.1 Sr 1.9 CaCu 2 O 8+x with Resonant Soft X-ray Scattering

Identifying what broken symmetries are present in the cuprates has become a major area of research. Many authors have reported evidence for so-called “Q ~ 0” order that involves broken inversion, mirror, chiral, or time-reversal symmetry that is uniform in space. Not all these observations are well understood and new experimental probes are needed. Here we use resonant soft x-ray scattering (RSXS) to search for Q ~ 0 order in Bi 2.1 Sr 1.9 CaCu 2 O 8+x (Bi-2212) by measuring the region of a forbidden Bragg peak, (0,0,3), which is normally extinguished by symmetry but may become allowed on resonance if valence band order is present. Using circularly polarized light, we found that this reflection becomes allowed on the CuL 3 resonance for temperatures T c < T < T*, though remains absent in linear polarization and at other temperatures. This observation suggests the existence of spatially uniform valence band order near the pseudogap temperature. In addition, we observed periodic oscillations in the specular reflectivity from the sample surface that resemble thin film interference fringes, though no known film is present. These fringes are highly resonant, appear in all polarizations, and exhibit a period that depends on the location where the beam strikes the sample surface. We speculate that these fringes arise from interaction between some intrinsic valence band instability and extrinsic structural surface morphologies of the material. Our study supports the existence of some kind of Q ~ 0 broken symmetry state in Bi-2212 at intermediate temperatures. Further studies using a microfocused beam, which could disentangle microscopic effects from macroscopic heterogeneities, are needed to ascertain the universality of the effect.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1996

Electronic Structure of TIBa(sub 2)CaCu(sub 2)O(sub 7-delta)

The core levels of TIBa(sub 2)CaCu(sub 2)O(sub 7-delta) epitaxial films have been measured with x-ray photoelectron spectroscopy (XPS). The valence electronic structure has been determined using the full-potential linear muffin tin orbital band structure method and measured with XPS.

Epitaxial films van Hove Fermi level↗
DOE OSTI2020

Materials Data on CaCu(GeO3)2 by Materials Project

CaCuGe2O6 is Esseneite structured and crystallizes in the monoclinic C2/c space group. The structure is three-dimensional. Ca2+ is bonded in a 8-coordinate geometry to eight O2- atoms. There are a spread of Ca–O bond distances ranging from 2.35–2.75 Å. Cu2+ is bonded to six O2- atoms to form CuO6 octahedra that share corners with six equivalent GeO4 tetrahedra and edges with two equivalent CuO6 octahedra. There are a spread of Cu–O bond distances ranging from 1.99–2.29 Å. Ge4+ is bonded to four O2- atoms to form GeO4 tetrahedra that share corners with three equivalent CuO6 octahedra and corners with two equivalent GeO4 tetrahedra. The corner-sharing octahedra tilt angles range from 45–61°. There are a spread of Ge–O bond distances ranging from 1.74–1.84 Å. There are three inequivalent O2- sites. In the first O2- site, O2- is bonded in a 2-coordinate geometry to two equivalent Ca2+ and two equivalent Ge4+ atoms. In the second O2- site, O2- is bonded in a 3-coordinate geometry to one Ca2+, one Cu2+, and one Ge4+ atom. In the third O2- site, O2- is bonded to one Ca2+, two equivalent Cu2+, and one Ge4+ atom to form a mixture of distorted edge and corner-sharing OCaCu2Ge tetrahedra.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on CaCu(GeO3)2 by Materials Project

CaCuGe2O6 crystallizes in the monoclinic P2_1/c space group. The structure is three-dimensional. Ca2+ is bonded in a 7-coordinate geometry to seven O2- atoms. There are a spread of Ca–O bond distances ranging from 2.35–2.69 Å. Cu2+ is bonded to six O2- atoms to form distorted CuO6 octahedra that share corners with three equivalent GeO4 tetrahedra, corners with two equivalent GeO5 trigonal bipyramids, edges with two equivalent CuO6 octahedra, and an edgeedge with one GeO5 trigonal bipyramid. There are a spread of Cu–O bond distances ranging from 1.94–2.52 Å. There are two inequivalent Ge4+ sites. In the first Ge4+ site, Ge4+ is bonded to four O2- atoms to form GeO4 tetrahedra that share corners with three equivalent CuO6 octahedra and corners with two equivalent GeO4 tetrahedra. The corner-sharing octahedra tilt angles range from 49–70°. There are a spread of Ge–O bond distances ranging from 1.73–1.82 Å. In the second Ge4+ site, Ge4+ is bonded to five O2- atoms to form GeO5 trigonal bipyramids that share corners with two equivalent CuO6 octahedra, corners with two equivalent GeO5 trigonal bipyramids, an edgeedge with one CuO6 octahedra, and an edgeedge with one GeO5 trigonal bipyramid. The corner-sharing octahedra tilt angles range from 40–50°. There are a spread of Ge–O bond distances ranging from 1.81–2.06 Å. There are six inequivalent O2- sites. In the first O2- site, O2- is bonded in a distorted rectangular see-saw-like geometry to one Ca2+, two equivalent Cu2+, and one Ge4+ atom. In the second O2- site, O2- is bonded to one Ca2+, two equivalent Cu2+, and one Ge4+ atom to form distorted corner-sharing OCaCu2Ge tetrahedra. In the third O2- site, O2- is bonded in a 4-coordinate geometry to two equivalent Ca2+ and two equivalent Ge4+ atoms. In the fourth O2- site, O2- is bonded in a trigonal planar geometry to one Ca2+ and two equivalent Ge4+ atoms. In the fifth O2- site, O2- is bonded in a 4-coordinate geometry to one Ca2+, one Cu2+, and two equivalent Ge4+ atoms. In the sixth O2- site, O2- is bonded in a distorted trigonal planar geometry to one Ca2+, one Cu2+, and one Ge4+ atom.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Discovery of orbital ordering in Bi 2 Sr 2 CaCu 2 O 8+x

The primordial ingredient of cuprate superconductivity is the CuO 2 unit cell. Theories usually concentrate on the intra-atom Coulombic interactions dominating the 3d 9 and 3d 10 configurations of each copper ion. However, if Coulombic interactions also occur between electrons of the 2p 6 orbitals of each planar oxygen atom, spontaneous orbital ordering may split their energy levels. This long-predicted intra-unit-cell symmetry breaking should generate an orbitally ordered phase, for which the charge transfer energy ε separating the 2p 6 and 3d 10 orbitals is distinct for the two oxygen atoms. Here we introduce sublattice-resolved ε(r) imaging to CuO 2 studies and discover intra-unit-cell rotational symmetry breaking of ε(r). Spatially, this state is arranged in disordered Ising domains of orthogonally oriented orbital order bounded by dopant ions, and within whose domain walls low-energy electronic quadrupolar two-level systems occur. Overall, these data reveal a Q = 0 orbitally ordered state that splits the oxygen energy levels by ~50 meV, in underdoped CuO 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Direct visualization of a static incommensurate antiferromagnetic order in Fe-doped Bi 2 Sr 2 CaCu 2 O 8+δ

Significance The pairing mechanism of high-temperature superconductivity, especially in cuprates, remains as the most challenging issue in condensed matter physics. The antiferromagnetic (AF) order/correlation is supposed to be important for inducing pairing and superconductivity. In this paper, we report the observation of a static incommensurate AF order by spin-polarized scanning tunneling microscope in Fe-doped Bi2212 with a nearly optimally doped state of superconductivity. The local incommensurate AF order can be directly visualized in regions with some Fe impurities. Our measurements provide a basis to study the interplay between superconductivity and AF spin fluctuations in cuprates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Revised phase diagram of the high- T c cuprate superconductor Pb-doped Bi 2 Sr 2 CaCu 2 O 8 + δ revealed by anisotropic transport measurements

Although phase diagrams can be leveraged to investigate high transition temperature (high-T c ) superconductivity, the issue has not been discussed thoroughly. In this study, we elucidate the phase diagram of the overdoped side of high-T c cuprates via systematic anisotropic transport measurements for Pb-doped Bi-2212 single crystals. We demonstrate that the characteristic temperatures of the “weak” pseudogap opening and electronic coherence cross each other at a critical doping level, while those of the “strong” pseudogap merges into that of superconducting fluctuations above the critical doping level. Her the results indicate the importance of Mottness in high-T c superconductivity.

36 MATERIALS SCIENCE↗