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At least 199 records · Page 11

Superconductivity in a quintuple-layer square-planar nickelate

Since the discovery of high-temperature superconductivity in the copper oxide materials, there have been sustained efforts to both understand the origins of this phase and discover new cuprate-like superconducting materials. One prime materials platform has been the rare-earth nickelates and indeed superconductivity was recently discovered in the doped compound Nd 0.8 Sr 0.2 NiO 2 . Undoped NdNiO 2 belongs to a series of layered square-planar nickelates with chemical formula Nd n+1 Ni n O 2n+2 and is known as the 'infinite-layer' (n=∞) nickelate. Furthermore, we report the synthesis of the quintuple-layer (n=5) member of this series, Nd 6 Ni 5 O 12 , in which optimal cuprate-like electron filling (d 8.8 ) is achieved without chemical doping. We observe a superconducting transition beginning at ~13 K. Electronic structure calculations, in tandem with magnetoresistive and spectroscopic measurements, suggest that Nd 6 Ni 5 O 12 interpolates between cuprate-like and infinite-layer nickelate-like behavior. In engineering a distinct superconducting nickelate, we identify the square-planar nickelates as a new family of superconductors which can be tuned via both doping and dimensionality.

36 MATERIALS SCIENCE↗

Evidence for d -wave superconductivity of infinite-layer nickelates from low-energy electrodynamics

The discovery of superconductivity in infinite-layer nickelates established another category of unconventional superconductors that shares structural and electronic similarities with cuprates. However, key issues of the superconducting pairing symmetry, gap amplitude and superconducting fluctuations are yet to be addressed. Here we utilize static and ultrafast terahertz spectroscopy to address these. We demonstrate that the equilibrium terahertz conductivity and non-equilibrium terahertz responses of an optimally Sr-doped nickelate film (superconducting transition temperature of T c = 17 K) are in line with the electrodynamics of d-wave superconductivity in the dirty limit. The gap-to-T c ratio (2Δ/k B T c ) is found to be 3.4, indicating that the superconductivity falls in the weak coupling regime. In addition, we observed substantial superconducting fluctuations near T c that do not extend into the deep normal state as the optimally hole-doped cuprates do. In conclusion, our results support a d-wave system that closely resembles the electron-doped cuprates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Emergence of quasiparticles in a doped Mott insulator

How a Mott insulator develops into a weakly coupled metal upon doping is a central question to understanding various emergent correlated phenomena. To analyze this evolution and its connection to the high- T c cuprates, we study the single-particle spectrum for the doped Hubbard model using cluster perturbation theory on superclusters. Starting from extremely low doping, we identify a heavily renormalized quasiparticle dispersion that immediately develops across the Fermi level, and a weakening polaronic side band at higher binding energy. The quasiparticle spectral weight roughly grows at twice the rate of doping in the low doping regime, but this rate is halved at optimal doping. In the heavily doped regime, we find both strong electron-hole asymmetry and a persistent presence of Mott spectral features. Finally, we discuss the applicability of the single-band Hubbard model to describe the evolution of nodal spectra measured by angle-resolved photoemission spectroscopy (ARPES) on the single-layer cuprate La 2– x Sr x CuO 4 (0 ≤ x ≤ 0.15). This work benchmarks the predictive power of the Hubbard model for electronic properties of high- T c cuprates.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Stripe correlations in the two-dimensional Hubbard-Holstein model

Several state-of-the-art numerical methods have observed static or fluctuating spin and charge stripes in doped two-dimensional Hubbard models, suggesting that these orders play a significant role in shaping the cuprate phase diagram. Many experiments, however, also indicate that the cuprates have strong electron-phonon (e-ph) coupling, and it is unclear how this interaction influences stripe correlations. We study static and fluctuating stripe orders in the doped single-band Hubbard-Holstein model using zero temperature variational Monte Carlo and finite temperature determinant quantum Monte Carlo. We find that the lattice couples more strongly with the charge component of the stripes, leading to an enhancement or suppression of stripe correlations, depending on model parameters like the next-nearest-neighbor hopping t' or phonon energy Ω. Our results help elucidate how the e-ph interaction can tip the delicate balance between stripe and superconducting correlations in the Hubbard-Holstein model with implications for our understanding of the high-T c cuprates.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Global phase diagram of D-wave superconductivity in the square-lattice t-J model

The Hubbard and closely related t-J models are exciting platforms for unconventional superconductivity (SC). Through state-of-the-art density matrix renormalization group calculations using the grand canonical ensemble, we address open issues regarding the ground-state phase diagram of the extended t-J model on a square lattice in the parameter regime relevant to cuprate superconductors. On large 8-leg cylinders, we demonstrate that the pure t-J model with only nearest-neighbor hoppings and superexchange interactions, for a wide range of doping ( δ = 0.1 to 0.2 ), hosts robust d-wave superconductivity possibly coexisting with weak unidirectional pair density wave. Furthermore, a small next nearest neighbor hopping t 2 suppresses pair and charge density waves, resulting in a uniform d-wave SC phase in both electron- and hole-doped cuprate model systems. Our work validates the t-J model as a proper minimum model for the emergence of superconductivity in cuprate superconductors.

Chen, Feng (ORCID:000000018196030X)↗

Evolution of the cyclotron mass with doping in La 2–x Sr x CuO 4

The recent observation of cyclotron resonance in optimally doped La 2–x Sr x CuO 4 using time-domain THz spectroscopy in high magnetic field has given new possibilities for the study of cuprate superconductors. One can measure the cyclotron mass in the more disordered cuprates possessing short scattering times, therefore expanding the study to materials and dopings in which quantum oscillations have not been observed. In this paper we present the measurement of the carrier mass of the hole-doped cuprate La 2–x Sr x CuO 4 across a range of dopings spanning from the slightly underdoped (p=0.13) to highly overdoped (p=0.26), near the termination of the superconducting dome. These results reveal a systematic increase of m c with doping, up to values greater than 13 times the bare electron mass. This is in contrast with the masses extracted from the heat capacity, which show a peak near the pseudogap critical point p* and/or Lifshitz transition. The cyclotron frequency is linear in field up to 31 T for all dopings, giving no evidence for field-induced Fermi surface reconstructions. The cyclotron mass is found to be positive for all dopings, but with a magnitude systematically below the heat-capacity mass for under and optimally doped samples, while exceeding it for overdoped samples. Among other aspects, these results are surprising as photoemission reveals a Lifshitz transition in the middle of our doping range and the sign of the cyclotron mass determined from a finite-frequency resonance is, in conventional theories, a topological quantity only sensitive to whether or not the Fermi surface is closed around holes or electrons. We see no sign of a divergence of the mass near p* nor near the Lifshitz transition, showing that any singularity, if it exists, is not strong enough to affect the cyclotron mass.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Strongly-overdoped $\mathrm{La}$ 2- $_{x}$$\mathrm{Sr}$$_{x}$$\mathrm{CuO}$ 4 : Evidence for Josephson-coupled grains of strongly-correlated superconductor

The interpretation of how superconductivity disappears in cuprates at large hole doping has been controversial. To address this issue, here we present an experimental study of single-crystal and thin film samples of La 2-x Sr x CuO 4 (LSCO) with x ≥0.25. In particular, measurements of bulk susceptibility on LSCO crystals with x = 0.25 indicate an onset of diamagnetism at T c1 =38.5 K, with a sharp transition to a phase with full bulk shielding at T c2 =18 K, independent of field direction. Strikingly, the in-plane resistivity only goes to zero at T c2 . Inelastic neutron scattering on 0.25 crystals confirms the presence of low-energy incommensurate magnetic excitations with reduced strength compared to lower doping levels. The ratio of the spin gap to T c2 is anomalously large. Our results are consistent with a theoretical prediction for strongly overdoped cuprates by Spivak, Oreto, and Kivelson, in which superconductivity initially develops within disconnected self-organized grains characterized by a reduced hole concentration, with bulk superconductivity occurring only after superconductivity is induced by proximity effect in the surrounding medium of higher hole concentration. Beyond the superconducting-to-metal transition, local differential conductance measurements on an LSCO thin film suggest that regions with pairing correlations survive, but are too dilute to support superconducting order. Future experiments will be needed to test the degree to which these results apply to overdoped cuprates in general.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Orbital polarization, charge transfer, and fluorescence in reduced-valence nickelates

Herein this paper presents a simple formalism for calculating X-ray absorption (XAS) and resonant inelastic x-ray scattering (RIXS) that has as input orbital-resolved density of states from a single particle or many-body ab initio calculation and is designed to capture itinerant-like features. We use this formalism to calculate both the XAS and RIXS with input from DFT and DFT + DMFT for the recently studied reduced valence nickelates R 4 Ni 3 O 8 and RNiO 2 (R = rare earth), and these results are then contrasted with those for the cuprate CaCuO 2 and the unreduced nickelate R 4 Ni 3 O 10 . In contrast to the unreduced R 4 Ni 3 O 10 , the reduced valence nickelates as well as the cuprate show strong orbital polarization due to the dominance of x 2 – y 2 orbitals for the unoccupied 3d states. We also reproduce two key aspects of a recent RIXS experiment for R 4 Ni 3 O 8 : (i) a charge transfer feature between 3d and oxygen 2p states whose energy we find to decrease as one goes from RNiO 2 to R 4 Ni 3 O 8 to the cuprate, and (ii) an energy-dependent polarization reversal of the fluorescence line that arises from hybridization of the unoccupied 3z 2 –r 2 states with R 5d states. We end with some implications of our results for the nature of the 3d electrons in reduced valence nickelates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Electronic structure, magnetic correlations, and superconducting pairing in the reduced Ruddlesden-Popper bilayer La 3 Ni 2 O 6 under pressure: Different role of d 3 z 2 - r 2 orbital compared with La 3 Ni 2 O 7

The recent discovery of superconductivity in bilayer La 3 Ni 2 O 7 (327-LNO) under pressure stimulated much interest in layered nickelates. However, superconductivity was not found in another bilayer nickelate system, La 3 Ni 2 O 6 (326-LNO), even under pressure. To understand the similarities and differences between 326-LNO and 327-LNO, using density functional theory and the random phase approximation (RPA), we systematically investigate 326-LNO under pressure. The large crystal-field splitting between the e g orbitals caused by the missing apical oxygen moves the d 3z 2 -r 2 orbital farther away from the Fermi level, implying that the d 3z 2 -r 2 orbital plays a less important role in 326-LNO than in 327-LNO. This also results in a smaller bandwidth for the d x 2 -y 2 orbital and a reduced energy gap for the bonding-antibonding splitting of the d 3z 2 -r 2 orbital in 326-LNO, as compared to 327-LNO. Moreover, the in-plane hybridization between the d x 2 -y 2 and d 3z 2 -r 2 orbitals is found to be small in 326-LNO, while it is much stronger in 327-LNO. Furthermore, the low-spin ferromagnetic state is found to be the likely ground state in 326-LNO under high pressure. The weak interlayer coupling suggests that s ± -wave pairing is unlikely in 326-LNO. The robust in-plane ferromagnetic coupling also suggests that d-wave superconductivity, which is usually caused by antiferromagnetic fluctuations of the d x 2 -y 2 orbital, is also unlikely in 326-LNO. These conclusions are supported by our many-body RPA calculations of the pairing behavior. Additionally, contrasting with the cuprates, for the bilayer cuprate HgBa 2 CaCu 2 O 6 , we find a strong self-doping effect of the d x 2 -y 2 orbital under pressure, with the charge of Cu being reduced by approximately 0.13 electrons from 0 GPa to 25 GPa. In contrast, we do not observe such a change in the electronic density in 326-LNO under pressure, establishing another important difference between the nickelates and the cuprates.

36 MATERIALS SCIENCE↗

Superconducting Dome in Nd 1-x Sr x NiO 2 Infinite Layer Films

We show the phase diagram of Nd 1-x Sr x NiO 2 infinite layer thin films grown on SrTiO 3 . A superconducting dome spanning 0.125 < x < 0.25 is found, remarkably similar to cuprates, albeit over a narrower doping window. However, while cuprate superconductivity is bounded by an insulator for underdoping and a metal for overdoping, here we observe weakly insulating behavior on either side of the dome. Furthermore, the normal state Hall coefficient is always small and proximate to a continuous zero crossing in doping and in temperature, in contrast to the ~ 1/x dependence observed for cuprates. This suggests the presence of both electronlike and holelike bands, consistent with band structure calculations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Soft X-Ray Spectroscopy of Low-Valence Nickelates

Low-valence nickelates—including infinite-layer (IL) and trilayer (TL) compounds—are longstanding candidates for mimicking the high-temperature superconductivity of cuprates. A recent breakthrough in the field came with the discovery of superconductivity in hole-doped IL nickelates. Yet, the degree of similarity between low-valence nickelates and cuprates is the subject of a profound debate for which soft x-ray spectroscopy experiments at the Ni L - and O K -edge provided critical input. In this review, we will discuss the essential elements of the electronic structure of low-valance nickelates revealed by x-ray absorption spectroscopy (XAS) and resonant inelastic x-ray scattering (RIXS). Furthermore, we will review magnetic excitations observed in the RIXS spectra of IL and TL nickelates, which exhibit characteristics that are partly reminiscent of those of cuprates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Hyperbolic Cooper-Pair Polaritons in Planar Graphene/Cuprate Plasmonic Cavities

Hyperbolic Cooper-pair polaritons (HCP) in cuprate superconductors are of fundamental interest due to their potential for providing insights into the nature of unconventional superconductivity. In this study, we critically assess an experimental approach using near-field imaging to probe HCP in Bi 2 Sr 2 CaCu 2 O 8+x (Bi-2212) in the presence of graphene surface plasmon polaritons (SPP). Our simulations show that inherently weak HCP features in the near-field can be strongly enhanced when coupled to graphene SPP in layered graphene/hexagonal boron nitride (hBN)/Bi-2212 heterostructures. This enhancement arises from our multilayered structures effectively acting as plasmonic cavities capable of altering collective modes of a layered superconductor by modifying its electromagnetic environment. The degree of enhancement can be selectively controlled by tuning the insulating spacer thickness with atomic precision. Finally, we verify the expected renormalization of room-temperature graphene SPP using near-field infrared imaging. Our modeling, augmented with data, attests to the validity of our approach for probing HCP modes in cuprate superconductors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Applying Configurational Complexity to the 2D Ruddlesden–Popper Crystal Structure

The layered Ruddlesden–Popper crystal structure can host a broad range of functionally important behaviors. In this work, we establish extraordinary configurational disorder in a layered Ruddlesden–Popper (RP) structure using entropy stabilization assisted synthesis. A protype A 2 CuO 4 RP cuprate oxide with five cations on the A-site sublattice is designed and fabricated into epitaxial single crystal films using pulsed laser deposition. When grown on a near lattice matched substrate, the (La 0.2 Pr 0.2 Nd 0.2 Sm 0.2 Eu 0.2 ) 2 CuO 4 film features a T'-type RP structure with uniform A-site cation mixing and square-planar CuO4 units. These observations are made with a range of combined characterizations using X-ray diffraction, atomic-resolution scanning transmission electron microscopy, energy-dispersive X-ray spectroscopy, and X-ray absorption spectroscopy measurements. It is further found that heteroepitaxial strain plays an important role in crystal phase formation during synthesis. Compressive strain over ~1.5% results in the formation of a non-RP cubic phase consistent with a Cu X 2O 4 spinel structure. The ability to manipulate configurational complexity and move between 2D layered RP and 3D cubic crystal structures in cuprate and related materials promises to enable flexible design strategies for a range of functionalities, such as magnetoresistance, unconventional superconductivity, ferroelectricity, catalysis, and ion transport.

36 MATERIALS SCIENCE↗

Local lattice distortions and dynamics in extremely overdoped superconducting YSr 2 Cu 2.75 Mo 0.25 O 7.54

A common characteristic of many “overdoped” cuprates prepared with high-pressure oxygen is T c values ≥ 50 K that often exceed that of optimally doped parent compounds, despite O stoichiometries that place the materials at the edge or outside of the conventional boundary between superconducting and normal Fermi liquid states. X-ray absorption fine-structure (XAFS) measurements at 52 K on samples of high-pressure oxygen (HPO) YSr 2 Cu 2.75 Mo 0.25 O 7.54 , T c = 84 K show that the Mo is in the (VI) valence in an unusually undistorted octahedral geometry with predominantly Mo neighbors that is consistent with its assigned substitution for Cu in the chain sites of the structure. Perturbations of the Cu environments are minimal, although the Cu X-ray absorption near-edge structure (XANES) differs from that in other cuprates. The primary deviation from the crystal structure is therefore nanophase separation into Mo- and Cu-enriched domains. There are, however, indications that the dynamical attributes of the structure are altered relative to YBa 2 Cu 3 O 7 , including a shift of the Cu-apical O two-site distribution from the chain to the plane Cu sites. Another effect that would influence T c is the possibility of multiple bands at the Fermi surface caused by the presence of the second phase and the lowering of the Fermi level.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Nonadiabatic coupling of the dynamical structure to the superconductivity in YSr 2 Cu 2.75 Mo 0.25 O 7.54 and Sr 2 CuO 3.3

A crucial issue in cuprates is the extent and mechanism of the coupling of the lattice to the electrons and the superconductivity. Here we report Cu K edge extended X-ray absorption fine structure measurements elucidating the internal quantum tunneling polaron (iqtp) component of the dynamical structure in two heavily overdoped superconducting cuprate compounds, tetragonal YSr 2 Cu 2.75 Mo 0.25 O 7.54 with superconducting critical temperature, T c = 84 K and hole density p = 0.3 to 0.5 per planar Cu, and the tetragonal phase of Sr 2 CuO 3.3 with T c = 95 K and p = 0.6. In YSr 2 Cu 2.75 Mo 0.25 O 7.54 changes in the Cu-apical O two-site distribution reflect a sequential renormalization of the double-well potential of this site beginning at T c , with the energy difference between the two minima increasing by ~6 meV between T c and 52 K. Sr 2 CuO 3.3 undergoes a radically larger transformation at T c , >1-Å displacements of the apical O atoms. The principal feature of the dynamical structure underlying these transformations is the strongly anharmonic oscillation of the apical O atoms in a double-well potential that results in the observation of two distinct O sites whose Cu–O distances indicate different bonding modes and valence-charge distributions. The coupling of the superconductivity to the iqtp that originates in this nonadiabatic coupling between the electrons and lattice demonstrates an important role for the dynamical structure whereby pairing occurs even in a system where displacements of the atoms that are part of the transition are sufficiently large to alter the Fermi surface. The synchronization and dynamic coherence of the iqtps resulting from the strong interactions within a crystal would be expected to influence this process.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Identification of a nematic pair density wave state in Bi 2 Sr 2 CaCu 2 O 8+x

Electron-pair density wave (PDW) states are now an intense focus of research in the field of cuprate correlated superconductivity. PDWs exhibit periodically modulating superconductive electron pairing that can be visualized directly using scanned Josephson tunneling microscopy (SJTM). Although from theory, intertwining the d-wave superconducting (DSC) and PDW order parameters allows a plethora of global electron-pair orders to appear, which one actually occurs in the various cuprates is unknown. In this work, we use SJTM to visualize the interplay of PDW and DSC states in Bi 2 Sr 2 CaCu 2 O 8+x at a carrier density where the charge density wave modulations are virtually nonexistent. Simultaneous visualization of their amplitudes reveals that the intertwined PDW and DSC are mutually attractive states. Then, by separately imaging the electron-pair density modulations of the two orthogonal PDWs, we discover a robust nematic PDW state. Its spatial arrangement entails Ising domains of opposite nematicity, each consisting primarily of unidirectional and lattice commensurate electron-pair density modulations. Further, we demonstrate by direct imaging that the scattering resonances identifying Zn impurity atom sites occur predominantly within boundaries between these domains. This implies that the nematic PDW state is pinned by Zn atoms, as was recently proposed [Lozano et al., Phys. Rev. B 103, L020502 (2021)]. Taken in combination, these data indicate that the PDW in Bi 2 Sr 2 CaCu 2 O 8+x is a vestigial nematic pair density wave state [Agterberg et al. Phys. Rev. B 91, 054502 (2015); Wardh and Granath arXiv:2203.08250].

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Fluctuating charge-density-wave correlations in the three-band Hubbard model

The high-temperature superconducting cuprates host unidirectional spin- and charge-density-wave orders that can intertwine with superconductivity in nontrivial ways. While the charge components of these stripes have now been observed in nearly all cuprate families, their detailed evolution with doping varies across different materials and at high and low temperatures. We address this problem using nonperturbative determinant quantum Monte Carlo calculations for the three-band Hubbard model. Using an efficient implementation, we can resolve the model’s fluctuating spin and charge modulations and map their evolution as a function of the charge transfer energy and doping. We find that the incommensurability of the charge modulations is decoupled from the spin modulations and decreases with hole doping, consistent with experimental measurements at high temperatures. These findings support the proposal that the high-temperature charge correlations are distinct from the intertwined stripe order observed at low-temperature and in the single-band Hubbard model.

42 ENGINEERING↗

Understanding the superconductivity and charge density wave interaction through quasi-static lattice fluctuations

In unconventional superconductors, coupled charge and lattice degrees of freedom can manifest in ordered phases of matter that are intertwined. In the cuprate family, fluctuating short-range charge correlations can coalesce into a longer-range charge density wave (CDW) order which is thought to intertwine with superconductivity, yet the nature of the interaction is still poorly understood. Here, by measuring subtle lattice fluctuations in underdoped YBa 2 Cu 3 O 6+y on quasi-static timescales (thousands of seconds) through X-ray photon correlation spectroscopy, we report sensitivity to both superconductivity and CDW. The atomic lattice shows remarkably faster relaxational dynamics upon approaching the superconducting transition at T c ≈ 65 K. By tracking the momentum dependence, we show that the intermediate scattering function almost monotonically scales with the relaxation distance of atoms away from their average positions above T c and in the presence of the CDW state, while this peculiar trend is reversed for other temperatures. These observations are consistent with an incipient CDW stabilized by local strain. This work provides insights into the crucial role of relaxational atomic fluctuations for understanding the electronic physics cuprates, which are inherently disordered due to carrier doping.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗