Abstract The occurrence of unconventional superconductivity in cuprates has long motivated the search for manifestations in other layered transition metal oxides. Recently, superconductivity is found in infinite‐layer nickelate (Nd,Sr)NiO2and (Pr,Sr)NiO2thin films, formed by topotactic reduction from the perovskite precursor phase. A topic of much current interest is whether rare‐earth moments are essential for superconductivity in this system. In this study, it is found that with significant materials optimization, substantial portions of the La1−xSrxNiO2phase diagram can enter the regime of coherent low‐temperature transport (x = 0.14 ‐ 0.20), with subsequent superconducting transitions and a maximum onset of ≈9 K atx = 0.20. Additionally, the unexpected indication of a superconducting ground state in undoped LaNiO2is observed, which likely reflects the self‐doped nature of the electronic structure. Combining the results of (La/Pr/Nd)1−xSrxNiO2reveals a generalized superconducting dome, characterized by systematic shifts in the unit cell volume and in the relative electron‐hole populations across the lanthanides.
more »
« less
Possible strain-induced enhancement of the superconducting onset transition temperature in infinite-layer nickelates
Abstract The mechanism of unconventional superconductivity in correlated materials remains a great challenge in condensed matter physics. The recent discovery of superconductivity in infinite-layer nickelates, as an analog to high-Tccuprates, has opened a new route to tackle this challenge. By growing 8 nm Pr0.8Sr0.2NiO2films on the (LaAlO3)0.3(Sr2AlTaO6)0.7substrate, we successfully raise the superconducting onset transition temperatureTcin the widely studied SrTiO3-substrated nickelates from 9 K into 15 K, which indicates compressive strain is an efficient protocol to further enhance superconductivity in infinite-layer nickelates. Additionally, the x-ray absorption spectroscopy, combined with the first-principles and many-body simulations, suggest a crucial role of the hybridization between Ni and O orbitals in the unconventional pairing. These results also suggest the increase ofTcbe driven by the change of charge-transfer nature that would narrow the origin of general unconventional superconductivity in correlated materials to the covalence of transition metals and ligands.
more »
« less
- Award ID(s):
- 2132338
- PAR ID:
- 10475980
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- Communications Physics
- Volume:
- 6
- Issue:
- 1
- ISSN:
- 2399-3650
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract Motivated by the recent observation of superconductivity withTc ~ 80 K in pressurized La3Ni2O71, we explore the structural and electronic properties ofA3Ni2O7bilayer nickelates (A = La-Lu, Y, Sc) as a function of pressure (0–150 GPa) from first principles including a Coulomb repulsion term. At ~ 20 GPa, we observe an orthorhombic-to-tetragonal transition in La3Ni2O7at variance with x-ray diffraction data, which points to so-far unresolved complexities at the onset of superconductivity, e.g., charge doping by variations in the oxygen stoichiometry. We compile a structural phase diagram that establishes chemical and external pressure as distinct and counteracting control parameters. We find unexpected correlations betweenTcand thein-planeNi-O-Ni bond angles for La3Ni2O7. Moreover, two structural phases with significantc+octahedral rotations and in-plane bond disproportionations are uncovered forA = Nd-Lu, Y, Sc that exhibit a pressure-driven electronic reconstruction in the Niegmanifold. By disentangling the involvement of basal versus apical oxygen states at the Fermi surface, we identify Tb3Ni2O7as an interesting candidate for superconductivity at ambient pressure. These results suggest a profound tunability of the structural and electronic phases in this novel materials class and are key for a fundamental understanding of the superconductivity mechanism.more » « less
-
Abstract A hallmark of many unconventional superconductors is the presence of many-body interactions that give rise to broken-symmetry states intertwined with superconductivity. Recent resonant soft X-ray scattering experiments report commensurate 3a0charge density wave order in infinite-layer nickelates, which has important implications regarding the universal interplay between charge order and superconductivity in both cuprates and nickelates. Here we present X-ray scattering and spectroscopy measurements on a series of NdNiO2+xsamples, which reveal that the signatures of charge density wave order are absent in fully reduced, single-phase NdNiO2. The 3a0superlattice peak instead originates from a partially reduced impurity phase where excess apical oxygens form ordered rows with three-unit-cell periodicity. The absence of any observable charge density wave order in NdNiO2highlights a crucial difference between the phase diagrams of cuprate and nickelate superconductors.more » « less
-
The local structure of the highly “overdoped” 95 K superconductor Sr2CuO3.3determined by Cu K X-ray absorption fine structure (XAFS) at 62 K in magnetically oriented samples shows that 1) the magnetization is perpendicular to thecaxis; 2) at these levels of precision the Cu sublattice is tetragonal in agreement with the crystal structure; the O sublattice has 3) continuous -Cu-O- chains that orient perpendicular to an applied magnetic field; 4) approximately half-filled -Cu-O- chains that orient parallel to this field; 5) a substantial number of apical O vacancies; 6) O ions at some apical positions with expanded Cu-O distances; and 7) interstitial positions that imply highly displaced Sr ions. These results contradict the universally accepted features of cuprates that require intact CuO2planes, magnetization along thecaxis, and a termination of the superconductivity when the excess charge on the CuO2Cu ions exceeds 0.27. These radical differences in charge and structure demonstrate that this compound constitutes a separate class of Cu-O–based superconductors in which the superconductivity originates in a different, more complicated structural unit than CuO2planes while retaining exceptionally high transition temperatures.more » « less
-
We report evidence for superconductivity with onset temperatures up to 11 K in thin films of the infinite-layer nickelate parent compound . A combination of oxide molecular beam epitaxy and atomic hydrogen reduction yields samples with high crystallinity and low residual resistivities, a substantial fraction of which exhibit superconducting transitions. We survey a large series of samples with a variety of techniques, including electrical transport, scanning transmission electron microscopy, x-ray absorption spectroscopy, and resonant inelastic x-ray scattering, to investigate the possible origins of superconductivity. We propose that superconductivity could be intrinsic to the undoped infinite-layer nickelates but suppressed by disorder due to a possibly sign-changing order parameter, a finding which would necessitate a reconsideration of the nickelate phase diagram. Another possible hypothesis is that the parent materials can be hole doped from randomly dispersed apical oxygen atoms, which would suggest an alternative pathway for achieving superconductivity. Published by the American Physical Society2025more » « less