The status of nickelate superconductors in relation to cuprate high temperature superconductors is one of the concepts being discussed in high temperature superconductivity in correlated transition metal oxides. New additions to the class of infinite layer nickelates can provide essential input relating to connections or distinctions. A recently synthesized compound Ba2NiO2(AgSe)2, which contains isolated ‘infinite layer’ NiO2planes, may lead to new insights. Our investigations have discovered that, at density functional theory mean field level, the ground state consists of an unusual
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-
- Award ID(s):
- 2132338
- NSF-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
-
more » « less
Abstract d 8anti-Hund’s singlet that emerges in this compound, and consider a minimally correlated wavefunction for this singlet in an itinerant background, and begin discussion of excitations—real or virtual—that may figure into new electronic phases. -
more » « less
Abstract Motivated by the recent observation of superconductivity with
T c ~ 80 K in pressurized La3Ni2O71, we explore the structural and electronic properties ofA 3Ni2O7bilayer 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 betweenT c and thein-plane Ni-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 Nie g manifold. 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 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−
x Srx NiO2phase 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−x Srx NiO2reveals a generalized superconducting dome, characterized by systematic shifts in the unit cell volume and in the relative electron‐hole populations across the lanthanides. -
We present a valence transition model for electron- and hole-doped cuprates, within which there occurs a discrete jump in ionicity Cu2+ -> Cu1+ in both families upon doping, at or near optimal doping in the conventionally prepared electron-doped compounds and at the pseudogap phase transition in the hole-doped materials. In thin films of the T' compounds, the valence transition has occurred already in the undoped state. The phenomenology of the valence transition is closely related to that of the neutral-to-ionic transition in mixed-stack organic charge-transfer solids. Doped cuprates have negative charge-transfer gaps, just as rare-earth nickelates and BaBiO3. The unusually high ionization energy of the closed shell Cu1+ ion, taken together with the dopingdriven reduction in three-dimensional Madelung energy and gain in two-dimensional delocalization energy in the negative charge transfer gap state drives the transition in the cuprates. The combined effects of strong correlations and small d-p electron hoppings ensure that the systems behave as effective 1/2-filled Cu band with the closed shell electronically inactive O2- ions in the undoped state, and as correlated two-dimensional geometrically frustrated 1/4-filled oxygen hole band, now with electronically inactive closed-shell Cu1+ ions, in the doped state. The model thus gives microscopic justification for the two-fluid models suggested by many authors. The theory gives the simplest yet most comprehensive understanding of experiments in the normal states. The robust commensurate antiferromagnetism in the conventional T' crystals, the strong role of oxygen deficiency in driving superconductivity and charge carrier sign corresponding to holes at optimal doping are all manifestations of the same quantum state. In the hole-doped pseudogapped state, there occurs a biaxial commensurate period 4 charge density wave state consisting of O1- -Cu l(1+)-O1- spin singlets that coexists with broken rotational C-4 symmetry due to intraunit cell oxygen inequivalence. Finite domains of this broken symmetry state will exhibit twodimensional chirality and the polar Kerr effect. Superconductivity within the model results from a destabilization of the 1/4-filled band paired Wigner crystal [Phys. Rev. B 93, 165110 (2016) and ihid. 93, 205111 (2016)]. We posit that a similar valence transition, Ir4+ -> Ir3+, occurs upon electron doping Sr2IrO4. We make testable experimental predictions in cuprates including superoxygenated La2CuO4+delta and iridates. Finally, as indirect evidence for the valence bond theory of superconductivity proposed here, we note that there exist an unusually large number of unconventional superconductors that exhibit superconductivity proximate to exotic charge ordered states, whose band fillings are universally 1/4 or 3/4, exactly where the paired Wigner crystal is most stable.more » « less
-
more » « less
Abstract The path from a Mott insulating phase to high temperature superconductivity encounters a rich set of unconventional phenomena involving the insulator-to-metal transition (IMT), such as emergent electronic orders and pseudogaps, that ultimately affect the condensation of Cooper pairs. A huge hindrance to understanding the origin of these phenomena is the difficulty in accessing doping levels near the parent state. The
J eff = 1/2 Mott state of the perovskite strontium iridates has revealed intriguing parallels to the cuprates, with the advantage that it provides unique access to the Mott transition. Here, we exploit this accessibility to study the IMT and the possible nearby electronic orders in the electron-doped bilayer iridate (Sr1 − xLax)3Ir2O7. Using spectroscopic imaging scanning tunneling microscopy, we image the La dopants in the top as well as the interlayer SrO planes. Surprisingly, we find a disproportionate distribution of La between these layers with the interlayer La being primarily responsible for the IMT. This reveals the distinct site-dependent effects of dopants on the electronic properties of bilayer systems. Electron doping also results in charge reordering. We find unidirectional electronic order concomitant with the structural distortion known to exist in this system. Intriguingly, similar to the single layer iridate, we also find local resonant states forming a checkerboard-like pattern trapped by La. This suggests that multiple charge orders may exist simultaneously in Mott systems, even with only one band crossing the Fermi energy.
