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Controlled introduction of oxygen vacancies offers an effective route to induce metal-to-insulator transition in strongly correlated rare-earth nickelates ($R$NiO$_3$) at room temperature. However, the role played by the rare-earth cations on the structure, thermodynamic stability, and electronic properties of oxygen-deficient nickelates remains unclear. Here, we employ density functional theory calculations with Hubbard corrections (DFT + $U$) to investigate the whole family of $R$NiO$_{2.5}$ ($R$ = Pr-Er) compounds in two commonly observed oxygen-vacancy ordered configurations, namely brownmillerite, and square planar. We find that square planar polymorph is always more stable ($\sim$0.4 eV/u.f) than the brownmillerite for all rare-earth cations, owing to the exceedingly low volumetric strains (< 1\%). Formation energy of $R$NiO$_{2.5}$ gradually increases with decreasing size of $R$ owing to stronger Ni-O covalent interactions in pristine $R$NiO$_3$ with small $R^{3+}$ cations. This necessitates more oxygen-lean environments for synthesis of $R$NiO$_{2.5}$ with smaller $R^{3+}$ cations. Analysis of the density of states and band structures reveals that electronic structure of $R$NiO$_{2.5}$ is governed by two factors: (a) localization of electron on NiO$_6$ octahedra yielding a Mott insulating state with strong correlations as Ni $e_g$ is half filled, and (b) crystal field splitting in the NiO$_4$ tetrahedra/square planar polyhedra. Brownmillerite $R$NiO$_{2.5}$ is metallic, while square planar $R$NiO$_{2.5}$ is an insulator with a predicted gap of $\sim$ 0.2-0.3 eV, depending on the $R^{3+}$ cation. Crystal orbital Hamilton population (COHP) analysis indicates that the Ni-O bond belonging to square-planar NiO$_4$ polyhedra exhibit much greater covalent character than those in NiO$_6$ octahedra in square planar $R$NiO$_{2.5}$.

Signatures of superconductivity under pressure have recently been reported in the bilayer La$_3$Ni$_2$O$_7$ and trilayer La$_4$Ni$_3$O$_{10}$ Ruddlesden-Popper (RP) nickelates with general chemical formula La$_{n+1}$Ni$_n$O$_{3n+1}$ ($n=$ number of perovskite layers along the $c$-axis). The emergence of superconductivity is always concomitant with a structural transition in which the octahedral tilts are suppressed causing an increase in the out-of-plane $d_{z^2}$ orbital overlap. Here, using first-principles calculations, we explore biaxial strain (both compressive and tensile) as a means to mimic the electronic structure characteristics of RP nickelates (up to $n=5$) under hydrostatic pressure. Our findings highlight that strain allows to decouple the structural and electronic structure effects obtained under hydrostatic pressure, with tensile strain reproducing the known electronic structure characteristics of the pressurized bilayer and trilayer compounds. Overall, strain represents a promising way to tune the electronic structure of RP nickelates and could be an alternative route to achieve superconductivity in this family of materials.

An important strategy for understanding the microscopic physics of strongly correlated systems and enhancing their technological potential is to selectively drive the fundamental degrees of freedom out of equilibrium. Intense terahertz (THz) pulses with photon energies of a few meV, can not only serve this purpose but also unravel their electronic and quantum nature. Here, we present THz-driven ultrafast dynamics of rare-earth nickelates $\text{RNiO}_{\text{3}}$, $\text{R}$ = rare-earth atom) - a prototype system to study the Mott insulator-metal transition (IMT). The THz drive of its Mott insulating state induces instantaneous IMT via quantum tunneling of valence electrons across the bandgap while the THz drive of its correlated metallic state leads to overall heating of the conduction electrons. The subsequent relaxations of excited electrons in these two states occur via a two-step process (electron-phonon thermalization and recovery of the charge-ordered insulating state) and a one-step process (electron-phonon scattering), respectively. The relaxation dynamics of the electrons and the absence of acoustic phonon modes, in particular, suggest that the THz photons drive only the charge degree of freedom. The purely electronic, ultrafast and local nature of the THz-induced IMT offers its applications in opto-electronics with enhanced performance and minimal device size and heat dissipation.

Motivated by the high temperature superconductivity observed in the bilayer nickelate La$_3$Ni$_2$O$_7$ and the spectroscopic evidences of strong electron correlations in this compound, we address the role of its multiorbital electron correlations by proposing a global phase diagram of a bilayer two-orbital Hubbard model. We find a Mott transition developing at half filling, and identify strong orbital selectivity when the system is at the physical electron count. The orbital selectivity is manifested in the formation of interlayer spin singlets between electrons in the $z^2$ orbitals. These features lead to a strong renormalization of the electronic band structure while sustaining a sizable splitting between the bonding and antibonding $z^2$ bands. The proposed orbital-selective correlations naturally explain a series of features as observed in the angular resolved photoemission spectroscopy (ARPES) and optical conductivity measurements in La$_3$Ni$_2$O$_7$. Our results provide a basis to understand both the normal state and the high temperature superconductivity of multilayer nickelates and thereby elucidate correlated superconductivity in general., Comment: 6+5 pages, 4+5 figures

We report on optical studies of the Ruddlesden-Popper nickelates La$_{n+1}$Ni$_{n}$O$_{3n+1}$ with $n = 2$ (La$_{3}$Ni$_{2}$O$_{7}$), $n = 3$ (La$_{4}$Ni$_{3}$O$_{10}$) and $n = \infty$ (LaNiO$_{3}$). As the number of the NiO$_{6}$ octahedra layers $n$ grows, the ratio of the kinetic energy determined from the experimental optical conductivity and that from band theory $K_{\text{exp}}/K_{\text{band}}$ increases, suggesting a reduction of electronic correlations. While the strong electronic correlations in the bilayer La$_{3}$Ni$_{2}$O$_{7}$ place it on the verge of the Mott insulating phase, the trilayer La$_{4}$Ni$_{3}$O$_{10}$ and infinite-layer LaNiO$_{3}$ exhibit moderate electronic correlations, falling into the regime of correlated metals. The evolution of the electronic correlations in La$_{n+1}$Ni$_{n}$O$_{3n+1}$ is likely to be dominated by the Ni-$d_{z^2}$ orbital. Our results provide important information for understanding the superconductivity in Ruddlesden-Popper nickelates., Comment: 7 pages, 4 figures. Comments are welcome and appreciated

Almost four decades of intense research have been invested to study the physics of high-T$_c$ cuprate superconductors. The recent discovery of high-T$_c$ superconductivity in pressurized bilayer nickelates and its potential similarities with cuprate superconductors may open a new window to understand this long standing problem. Motivated by this we have assumed that nickelates belong to the category of strongly correlated systems, and considered the bilayer $t$-$J_\parallel$-$J_\perp$ model as a minimal model, where $J_\parallel$ and $J_\perp$ are the in-plane and out-of-plane magnetic exchange, respectively. We have studied the $t$-$J_\parallel$-$J_\perp$ model in a large-$N$ approach on the basis of the path integral representation for Hubbard operators, which allows to obtain results at mean-field and beyond mean-field level. We find that $J_\perp$ is a promising candidate for triggering high superconducting $T_c$ values at quarter filling (hole doping $\delta=0.5$) of the $d_{x^2-y^2}$ orbitals. Beyond mean-field level, we remarkably find a new phase, an out-of-plane bond-order phase (z-BOP), triggered also by $J_\perp$. z-BOP develops below a critical temperature which decreases with increasing doping and vanishes at a quantum critical point below quarter filling. The occurrence of this phase and its competition with superconductivity leads to a superconducting dome shaped behavior as a function of doping and as a function of $J_\perp$. Comparisons with the physics of cuprates and the recent literature on the new pressurized nickelates are given along the paper., Comment: 7 pages (main text) + 8 pages (references + appendices), 7 figures

Characterizing the dimensionality of the superconducting state in the infinite-layer (IL) nickelates is crucial to understand its nature. Most studies have addressed the problem by studying the anisotropy of the upper critical fields. Yet, the dominance of Pauli-paramagnetism effects over orbital ones makes it challenging to interpret the experiments in terms of dimensionality. Here we address the question from a different perspective, by investigating the vortex phase diagram in the mixed-state. We demonstrate that superconducting Pr0.8Sr0.2NiO2 thin films present a vortex liquid-to-glass transition of a purely two-dimensional nature. The obtained results suggest that bidimensionality is an intrinsic property, and that superconductivity resides in fully-decoupled NiO2 planes. In this scenario, the coherence length along the c-axis must be shorter than the distance between those planes, while Josephson and magnetostatic coupling between them must be negligible. We believe that these conclusions are relevant for theories on the origin of superconductivity in the IL-nickelates.

While key attention in transition-metal oxides is usually devoted to the $d$ states of the transition-metal ion, the O$(2p)$ states usually also carry important physics. We here examine these $p$ states in representatives of the novel superconducting nickelates, as described in realistic dynamical mean-field theory. Since the materials are located on the boundary between Mott-Hubbard and charge-transfer systems, the role of oxygen is expectedly subtle. Strong reduction of doped holes on oxygen and first asymmetry effects are featured in infinite-layer nickelates. A pronounced nature of bridging $p_z$ orbitals is identified in the La$_3$Ni$_2$O$_7$ system., Comment: 10 pages

We report a comprehensive study of electronic band structure for single-layer (SL) and bilayer (BL) RP-nickelates probed by in-situ HP X-ray absorption near edge spectroscopy (XANES). At ambient pressure (AP), the energy splitting delta_E of d_3z^2-r^2 and d_x^2-y^2 bands are directly observed in La3Ni2O7 (BL-La327) but not in La2NiO4 (SL-La214) above E_F, underlining the critical role of inner apical O atoms. A combination of DFT-based electronic band structure and projected density of states (PDOS) calculations with simulated XANES enables us to explain the observed main XANES features labelled by a, A, B', B and C when considering the orbital hybridizations, crystal field splitting (CFS) and core-hole screening of different 3d configurations for SL-La214 and BL-La327 nickelates. At high pressure (HP), the delta_E values of pre-edge peak form a dome-like evolution above 7.7 GPa with the maximum locating at around 20 GPa for metallic BL-La327. Analysis of its integrated area and FWHM provides strong evidence that the bonding d_3z^2-r^2 band crosses E_F above about 7.7 GPa for the metallic BL-La327. Growth of integrated area of pre-edge peak and C peak further evidences pressure-induced hole doping effect. Meanwhile, the pressure dependent FWHM of pre-edge peak implies a nonmonotonic evolution of orbital-selective electronic correlation above 7.7 GPa with extrema emerging at about 20 GPa. Moreover, we estimate the relative hole doping level using the energy shift of pre-edge peak, yielding 0.074 hole per Ni site or equivalently 1.1*10^21 cm^-3 at 20 GPa for the metallic BL-La327, which is comparable to cuprates. Our results have timely examined the electronic band structures as obtained from theoretical calculations, emphasizing the essential role of both d_3z^2-r^2 and d_x^2-y^2 bands as well as the electronic correlation in superconducting pairing for pressurized La3Ni2O7.

Recently discovered superconducting infinite-layer nickelates $R$NiO$_2$ ($R$=Nd, La, Pr) attract increasing attention due to the similarites to cuprates. Both $R$NiO$_2$ and YBCO cuprates exhibit the non-fermi-liquid transport behavior, characterized by resistivity proportional to temperature near the quantum critical point of the charge or spin density wave. In this study, we analyze the resistivity of infinite-layer nickelate Nd$_{0.85}$Sr$_{0.15}$NiO$_2$ based on a three-dimensional tight-binding model by applying linear response theory. We take account of the self-energy by the fluctuation exchange (FLEX) approximation for the Ni orbital and the T-matrix approximation for an impurity effect on the Nd orbitals. We find that (i) the $T$-linear resistivity at low temperatures is derived from the spin fluctuations, and (ii) a negative and $T$-linear Seebeck coefficient is obtained. The resulting $T$-linear resistivity suggests that NdNiO$_2$ behaves as a quasi-two-dimensional electron system similar to CeCoIn$_5$., Comment: 5 pages, 7 figures

Based on the energy level structure of neutral oxygen atom O and its anions, through in-depth analysis of the bonding process and formation mechanism of anion O$^{x-}$ ($1

Rare-earth orthonickelates RNiO3 are Jahn-Teller magnets, unstable with respect to the anti-Jahn-Teller disproportionation reaction with the formation of a system equivalent to a system of effective spin-triplet composite bosons moving in a non-magnetic lattice. Within the framework of the two-sublattice approximation, we have developed a mean field theory for a model nickelate with competition between phases of charge ordering, an antiferromagnetic insulator and a spin-triplet superconductor, and constructed phase diagrams taking into account phase separation.

Several reports about infinite-layer nickelate thin films suggest that the superconducting critical temperature versus chemical doping phase diagram has a dome-like shape, similar to cuprates. Here, we demonstrate a highly reproducible superconducting state in undoped PrNiO$_2$ thin films grown onto SrTiO$_3$. Scanning transmission electron microscopy measurements demonstrate coherent and defect-free infinite-layer phase, a high structural quality with no unintentional chemical doping and a total absence of interstitial oxygen. X-ray absorption measurements show very sharp features at the Ni L$_{3,2}$-edges with a large linear dichroism, indicating the preferential hole-occupation of Ni$^{1+}$-3d$_{x^2-y^2}$ orbitals in a square planar geometry. Resonant inelastic X-ray scattering measurements reveal sharp magnon excitations of 200\,meV energy at magnetic Brillouin zone boundary, highly resonant at the Ni$^{1+}$ absorption peak. The results indicate that, when properly stabilized, infinite-layer nickelate thin films are superconducting without chemical doping.

The discovery of the superconductivity in the infinite-layer nickelates, as topotactically reduced from their respective perovskite percussors via co-annealing with CaH2, extends the understanding in superconductivity. Nevertheless, whether the incorporated 1H composition is critical to the infinite-layer superconductivity recently arouses considerable debates, while the central challenge lies in the quantification of 1H that is easily interfered by the conventional electron or orbital associated processes. Herein, we demonstrate the irrelevance between the superconductivity in the infinite-layer nickelates and their incorporated 1H composition, assisted by nuclear reaction analysis (NRA) and heavy ion energy recoil detection analysis (HIERDA) based on the nuclear interactions at MeV energy scale. These approaches completely overwhelm the conventional interferes, such as ionization, activation and chemical bonds, and achieves the 1H quantification within superconducting La0.8Sr0.2NiO2 (or Nd0.8Sr0.2NiO2). A large diversity of 1H composition far beyond the previously expected critical dome was observed, while their TC were not changed significantly. Furthermore, the superconductivity was demonstrated to be achievable for La0.8Sr0.2NiO2 reduced by Al without any hydrogen associated process, while the superconducting properties for the CaH2 reduced La0.8Sr0.2NiO2 is rather stable after long term exposure in air, despite the high volatility of 1H within oxides. All these results indicate that the 1H incorporation composition is not critical to the superconductivity of the infinite-layer nickelates.

The observation of high-$T_c$ superconductivity (HTSC) in concomitant with pressure-induced orthorhombic-tetragonal structural transition in the bilayer La$_{3}$Ni$_2$O$_7$ has sparked hopes of achieving HTSC by stabilizing the tetragonal phase at ambient pressure. To mimic the effect of external physical pressures, the application of chemical pressure via replacing La$^3$$^+$ with smaller rare-earth R$^3$$^+$ has been considered as a potential route. Here we clarify the distinct effects of chemical and physical pressures on the structural transition of bilayer nickelates through a combined experimental and theoretical investigation. Contrary to general expectations, we find that substitutions of smaller R$^3$$^+$ for La$^3$$^+$ in La$_{3-x}$R$_x$Ni$_2$O$_{7-\delta}$, despite of an overall lattice contraction, produce stronger orthorhombic structural distortions and thus require higher pressures to induce the structural transition. We established a quantitative relationship between the critical pressure $P_c$ for structural transition and the average size of $A$-site cations. A linear extrapolation of $P_c$ versus <$r_A$> yields a putative critical value of <$r_A$>$_c$ ~ 1.23 angstrom for $P_c$ ~ 1 bar. The negative correlation between $P_c$ and <$r_A$> indicates that it is unlikely to reduce $P_c$ to ambient by replacing La$^3$$^+$ with smaller R$^3$$^+$ ions. Instead, partial substitution of La$^3$$^+$ with larger cations such as alkaline-earth Sr$^2$$^+$ or Ba$^2$$^+$ might be a feasible approach. Our results provide valuable guidelines in the quest of ambient-pressure HTSC in bilayer nickelates., Comment: 17 pages and 5 figures

Layered Nickelates have gained intensive attention as potential high-temperature superconductors, showing similarities and subtle differences to well-known Cuprates. This study introduces a modelling framework to analyze the tunability of electronic structures by focusing on effective orbitals and additional Fermi pockets, mimicking doping or external pressure qualitatively. It investigates the role of the $3d_{z^2}$ orbital in interlayer hybridization, which leads to the formation of a second pocket in the Fermi surface. The resulting effective model also predicts specific charge and spin susceptibility in the form of Lindhard susceptibility at wave vector $\mathbf{q_{0}} = (\pi, \pi)$, which can be tuned by doping or pressure. These results provide valuable insights into tunable orbital contributions and their influence on potential ordering and electronic instabilities in Layered Nickelates.

The relative role of electron-electron and electron-lattice interactions in driving the metal-insulator transition in perovskite nickelates opens a rare window into the non-trivial interplay of the two important degrees of freedom in solids. The most promising solution is to extract the electronic and lattice contributions during the phase transition by performing high-resolution spectroscopy measurements. Here, we present a three-dimensional electronic structure study of Nd1-xSrxNiO3 (x = 0 and 0.175) thin films with unprecedented accuracy, in which the low energy fermiology has a quantitative agreement with model simulations and first-principles calculations. Two characteristic phonons, the octahedral rotational and breathing modes, are illustrated to be coupled with the electron dynamics in the metallic phase, showing a kink structure along the band dispersion, as well as a hump feature in the energy spectrum. Entering the insulating state, the electron-phonon interaction is amplified by strong electron correlations, transforming the mobile large polarons at high temperatures to localized small polarons in the ground state. Moreover, the analysis of quasiparticle residue enables us to establish a transport-spectroscopy correspondence in Nd1-xSrxNiO3 thin films. Our findings demonstrate the essential role of electron-lattice interaction enhanced by the electronic correlation to stabilize the insulating phase in the perovskite nickelates., Comment: 26 pages, 4 + 7 figures

Within a Hubbard model, we investigate the superconducting pairing behavior of infinite-layer nickelate $\mathrm{NdNiO_2}$ and cuprate superconductors by using the determinant quantum Monte Carlo method. Our focus is on comparing their dominant pairing symmetries. The results indicate that the $d_{x^2-y^2}$ pairing interaction is significantly enhanced at low temperatures in both doped nickelates and cuprates, whereas other typical pairing symmetries are effectively suppressed, highlighting the dominance of the $d_{x^2-y^2}$ pairing form. Additionally, we find that the effective pairing interaction for $d_{x^2-y^2}$ pairing in doped nickelates is slightly lower than that in doped cuprates, which may be attributed to the different degrees of Fermi surface warping caused by the third-nearest hopping $t''$. Further studies show that the hole doping and interaction strength have significant effects on the $d_{x^2-y^2}$ pairing interaction within the selected parameter range. The $d_{x^2-y^2}$ pairing interaction is notably weakened when the hole doping increases, whereas it is significantly enhanced with increasing Coulomb interaction strength $U$. This comparative analysis reveals the similarities and differences in the pairing behaviors of doped nickelates and cuprates, which may provide further insights into understanding the superconducting properties of these two classes of materials., Comment: 8 pages and 12 figures. Published version

In rare earth nickelates (RENiO$_3$), electron-lattice coupling drives a concurrent metal-to-insulator and bond disproportionation phase transition whose microscopic origin has long been the subject of active debate. Of several proposed mechanisms, here we test the hypothesis that pairs of self-doped ligand holes spatially condense to provide local spin moments that are antiferromagnetically coupled to Ni spins. These singlet-like states provide a basis for long-range bond and spiral spin order. Using magnetic resonant X-ray scattering on NdNiO$_3$ thin films, we observe the chiral nature of the spin-disproportionated state, with spin spirals propagating along the crystallographic (101)$_\mathrm{ortho}$ direction. These spin spirals are found to preferentially couple to X-ray helicity, establishing the presence of a hitherto-unobserved macroscopic chirality. The presence of this chiral magnetic configuration suggests a potential multiferroic coupling between the noncollinear magnetic arrangement and improper ferroelectric behavior as observed in prior studies on NdNiO$_3$ (101)$_\mathrm{ortho}$ films and RENiO$_3$ single crystals. Experimentally constrained theoretical double-cluster calculations confirm the presence of an energetically stable spin-disproportionated state with Zhang-Rice singlet-like combinations of Ni and ligand moments., Comment: 6 pages, 4 figures

We theoretically propose a possibility of realizing high $T_c$ superconductivity having $s\pm$-wave symmetry in the heavily hole-doped infinite layer nickelates La$_{1-x}$Sr$_x$NiO$_2$. We consider situations where the original $P4/mmm$ symmetry of LaNiO$_2$ is maintained even for a significant amount of Sr substitution by growing thin films on substrates having tetragonal symmetry. Considering such cases is indeed justified by our phonon calculations. For electron configurations somewhat close to $d^8$, the interaction between the $d_{x^2-y^2}$ band and the other $3d$ bands that lie just below the Fermi level results in an enhancement of superconductivity where the sign of the gap function is reversed between the former and the latter bands. The strong enhancement of superconductivity can be attributed to the large energy level offset between $d_{x^2-y^2}$ and other orbitals due to the absence of the apical oxygens, as has been pointed out in previous studies., Comment: 4 pages, 4 figures

Conflicting theoretical scenarios for infinite-layer nickelate superconductors have been hotly debated, particularly regarding whether {only} a single Ni-3$d_{x^2-y^2}$ band is relevant at low energies besides electron pockets or whether multi-orbital physics including Ni-3$d_{z^2}$ is instead essential. The first scenario has emerged from density-functional theory plus dynamical mean-field theory (DFT+DMFT) calculations. Comparing the previous DFT+DMFT spectra to recent angular-resolved photoemission spectroscopy (ARPES) experiments, we find excellent agreement for both the Fermi surface and the strongly renormalized quasi-particle bands, supporting the first scenario. Our key findings further suggest that the "waterfalls" observed in ARPES might emerge from the quasi-particle--to--Hubbard-band crossover, and that additional spectral weight close to the $A$-pocket {likely} originates from the Ni-3$d_{xy}$ orbital., Comment: 8 pages, 4 figures

Motivated by the recently discovered high-$T_c$ bilayer nickelate superconductor La$_3$Ni$_2$O$_7$, we comprehensively research a bilayer $2\times2\times2$ cluster for different electronic densities $n$ by using the Lanczos method. We also employ the random-phase approximation to quantify the first magnetic instability with increasing Hubbard coupling strength, also varying $n$. Based on the spin structure factor $S(q)$, we have obtained a rich magnetic phase diagram in the plane defined by $n$ and $U/W$, at fixed Hund coupling. We have observed numerous states, such as A-AFM, Stripes, G-AFM, and C-AFM. For half-filling $n=2$ (two electrons per Ni site, corresponding to $N$ = 16 electrons), the canonical superexchange interaction leads to a robust G-AFM state $(\pi,\pi,\pi)$ with antiferromagnetic couplings in plane and between layers. By increasing or decreasing electronic densities, ferromagnetic tendencies emerge from the ``half-empty'' and ``half-full'' mechanisms, leading to many other interesting magnetic tendencies. In addition, the spin-spin correlations become weaker both in the hole or electron doping regions compared with half-filling. At $n = 1.5$ (or $N=12$), density corresponding to La$_3$Ni$_2$O$_7$, we obtained the ``Stripe 2'' ground state (antiferromagnetic coupling in one in-plane direction, ferromagnetic coupling in the other, and antiferromagnetic coupling along the $z$-axis) in the $2\times2\times2$ cluster. In addition, we obtained a much stronger AFM coupling along the $z$-axis than the magnetic coupling in the $xy$ plane. The random-phase approximation calculations with varying $n$ give very similar results as Lanczos. Meanwhile, a state with $q/\pi = (0.6, 0.6, 1)$ close to the E-phase wavevector is found in our RPA calculations by slightly reducing the filling to $n=1.25$, possibly responsible for the E-phase SDW recently observed in experiments., Comment: 12 pages, 9 figures

The discovery of nickelate superconductivity provided the first example of a non-copper-based material with superconductivity strongly analogous to the cuprates, but recent findings raise questions and inconsistencies around the electron counts and doping phase diagrams. We show using superconducting La$_4$Ni$_3$O$_{10}$ that there are unconventional interlayer and interorbital intrinsic doping effects that render the $d_{x^2-y^2}$ orbital occupation similar to the cuprates. The results enable a consistent framework for nickelate superconductivity, while maintaining the connection between cuprate and nickelate superconductors.

The superconducting infinite-layer (IL) nickelates offer a new platform for investigating the long-standing problem of high-temperature superconductivity. Many models were proposed to understand its superconducting mechanisms based on the calculated electronic structure, and the multiple Fermi surfaces and multiple orbitals involved create complications and controversial conclusions. Over the past 5 years, the lack of direct measurements of the electronic structure has hindered the understanding of nickelate superconductors. Here we fill this gap by directly resolving the electronic structures of the parent compound LaNiO$_2$ and superconducting La$_{0.8}$Ca$_{0.2}$NiO$_2$ using angle-resolved photoemission spectroscopy (ARPES). We find that their Fermi surfaces consist of a quasi-two-dimensional (quasi-2D) hole pocket and a three-dimensional (3D) electron pocket at the Brillouin zone corner, whose volumes change upon Ca doping. The Fermi surface topology and band dispersion of the hole pocket closely resemble those observed in hole-doped cuprates. However, the cuprate-like band exhibits significantly higher hole doping in superconducting La$_{0.8}$Ca$_{0.2}$NiO$_2$ compared to superconducting cuprates, highlighting the disparities in the electronic states of the superconducting phase. Our observations highlight the novel aspects of the IL nickelates, and pave the way toward the microscopic understanding of the IL nickelate family and its superconductivity., Comment: 12 pages, 4 figures

Revealing the momentum-resolved electronic structure of infinite-layer nickelates is essential for understanding this new class of unconventional superconductors, but has been hindered by the formidable challenges in improving the sample quality. In this work, we report for the first time the angle-resolved photoemission spectroscopy of superconducting La$_{0.8}$Sr$_{0.2}$NiO$_{2}$ films prepared by molecular beam epitaxy and ${\mathrm{\textit{in situ}}}$ atomic-hydrogen reduction. The measured Fermi topology closely matches theoretical calculations, showing a large Ni-$d_{x^2-y^2}$ derived Fermi sheet that evolves from hole-like to electron-like along $k_{z}$, and a three-dimensional (3D) electron pocket centered at Brillouin zone corner. The Ni-$d_{x^2-y^2}$ derived bands show a mass enhancement ($m^*/m_{\rm{DFT}}$) of 2-3,while the 3D electron band shows negligible band renormalization. Moreover, the Ni-$d_{x^2-y^2}$ derived states also display a band dispersion anomaly at higher binding energy, reminiscent of the waterfall feature and kinks observed in cuprates., Comment: 29 pages,13 figures

Motivated by the discovery of superconductivity in infinite-layer nickelates RNiO$_2$ (R= rare-earth), and the subsequent enhancement of their T$_c$ with pressure, we investigate the evolution of the electronic structure and magnetic properties of this family of materials via first-principles calculations employing hydrostatic and chemical pressure as tuning knobs. Overall, our analysis shows that pressure tends to increase the R-$5d$ self-doping effect, as well as the Ni-$d _{x^{2}-y^{2}}$ bandwidth, the $e_g$ energy splitting, the charge transfer energy, and the superexchange ($J$). Using the energy scale of $J$ as a predictor of superconducting tendencies, we anticipate that pressure can indeed be a feasible means to further increase the T$_c$ in this family of materials., Comment: 12 pages, 11 figures

A key open question in the study of layered superconducting nickelate films is the role that hydrogen incorporation into the lattice plays in the appearance of the superconducting state. Due to the challenges of stabilizing highly crystalline square planar nickelate films, films are prepared by the deposition of a more stable parent compound which is then transformed into the target phase via a topotactic reaction with a strongly reducing agent such as CaH$_2$. Recent studies, both experimental and theoretical, have introduced the possibility that the incorporation of hydrogen from the reducing agent into the nickelate lattice may be critical for the superconductivity. In this work, we use secondary ion mass spectrometry to examine superconducting La$_{1-x}$X$_x$NiO$_2$ / SrTiO$_3$ (X = Ca and Sr) and Nd$_6$Ni$_5$O$_{12}$ / NdGaO$_3$ films, along with non-superconducting NdNiO$_2$ / SrTiO$_3$ and (Nd,Sr)NiO$_2$ / SrTiO$_3$. We find no evidence for extensive hydrogen incorporation across a broad range of samples, including both superconducting and non-superconducting films. Theoretical calculations indicate that hydrogen incorporation is broadly energetically unfavorable in these systems, supporting our conclusion that hydrogen incorporation is not generally required to achieve a superconducting state in layered square-planar nickelates., Comment: 23 pages, 21 figures (including supplemental information)

Topotactic reduction utilizing metal hydrides as reagents emerges as an effective approach to achieve exceptionally low oxidization states of metal ions and unconventional coordination networks. This method opens avenues to the development of entirely new functional materials, with one notable example being the infinite-layer nickelate superconductors. However, the reduction effect on the atomic reconstruction and electronic structures -- crucial for superconductivity -- remains largely unresolved. We design two sets of control Nd$_{0.8}$Sr$_{0.2}$NiO$_2$ thin films and implement secondary ion mass spectroscopy to highlight the absence of reduction-induced hydrogen intercalation. X-ray absorption spectroscopy shows a significant linear dichroism with dominant Ni 3d$_{x2{-}y2}$ orbitals on superconducting samples, indicating a Ni single-band nature of infinite-layer nickelates. Consistent with the superconducting $T_c$, the Ni 3d orbitals asymmetry manifests a dome-like reduction duration dependence. Our results unveil the critical role of reduction in modulating the Ni-3d orbital polarization and its impact on the superconducting properties., Comment: Main: 21 pages, 4 figure - Supplementary: 7 pages, 5 figure

The formation of plasmons through the collective excitation of charge density has generated intense discussions, offering insights to fundamental sciences and potential applications. While the underlying physical principles have been well-established, the effects of many-body interactions and orbital hybridization on plasmonic dynamics remain understudied. In this work, we present the observation of conventional metallic and correlated plasmons in epitaxial La1-xSrxNiO3 (LSNO) films with varying Sr doping concentrations (x = 0, 0.125, 0.25), unveiling their intriguing evolution. Unlike samples at other doping concentrations, the x = 0.125 intermediate doping sample does not exhibit the correlated plasmons despite showing high optical conductivity. Through a comprehensive experimental investigation using spectroscopic ellipsometry and X-ray absorption spectroscopy, the O2p-Ni3d orbital hybridization for LSNO with a doping concentration of x = 0.125 is found to be significantly enhanced, alongside a considerable weakening of its effective correlation U*. These factors account for the absence of correlated plasmons and the high optical conductivity observed in LSNO (0.125). Our results underscore the profound impact of orbital hybridization on the electronic structure and the formation of plasmon in strongly-correlated systems. This in turn suggest that LSNO could serve as a promising alternative material in optoelectronic devices.

Motivated by the recently proposed alternating single-layer trilayer stacking structure for the nickelate La$_3$Ni$_2$O$_7$, we comprehensively study this system using {\it ab initio} and random-phase approximation techniques. Our analysis unveils similarities between this novel La$_3$Ni$_2$O$_7$ structure and other Ruddlesden-Popper nickelate superconductors, such as a similar charge-transfer gap value and orbital-selective behavior of the $e_g$ orbitals. However, different from other Ruddlesden-Popper nickelate superconductors, we do not observe any obvious reconstruction of the Fermi surface from ambient conditions (Cmmm phase) to high pressures (P4/mmm phase). Pressure primarily increases the bandwidths of the Ni $e_g$ bands, suggesting an enhancement of the itinerant properties of those $e_g$ states. Furthermore, the $d_{3z^2-r^2}$ orbital also has a layer-selective behavior because the antibonding-bonding-nonbonding splitting can only be obtained in the trilayer. In addition, we observe a "self-doping" effect from the trilayer to the single-layer sublattices and this effect will be enhanced by overall electron doping. Moreover, we find a leading $d_{x^2-y^2}$-wave pairing state that is restricted to the single-layer. Because the effective coupling between the single layers is very weak -- due to the non-superconducting trilayer in between -- this suggests that the superconducting transition temperature $T_c$ in this structure should be much lower than in the bilayer structure., Comment: 8 Pages 4 figure

The recent observation of high-T$_c$ superconductivity in the bilayer nickelate La$_3$Ni$_2$O$_7$ under pressure has garnered significant interests. While researches have predominantly focused on the role of electron-electron interactions in the superconducting mechanism, the impact of electron-phonon coupling (EPC) has remained elusive. In this work, we perform first-principles calculations to study the phonon spectrum and electron-phonon coupling within La$_3$Ni$_2$O$_7$ under pressure and explore of the interplay between EPC and electronic interactions on the superconductivity by employing functional renormalization group approach. Our calculations reveal that EPC alone is insufficient to trigger superconductivity in La$_3$Ni$_2$O$_7$ under pressure. We identify unique out-of-plane and in-plane breathing phonon modes which selectively couple with the Ni $d_{z^2}$ and $d_{x^2-y^2}$ orbitals, showcasing an orbital-selective EPC. Within the bilayer two-orbital model, it is revealed that solely electronic interactions foster $s_{\pm}$-wave pairing characterized by notable frustration in the band space, leading to a low transition temperature. Remarkably, we find that this out-of-plane EPC can act in concert with electronic interactions to promote the onsite and interlayer pairing in the $d_{z^2}$ orbital, partially releasing the pairing frustration and thus elevating T$_c$. In contrast, the inclusion of in-plane EPC only marginally affects the superconductivity, distinct from the cuprates. Potential experimental implications in La$_3$Ni$_2$O$_7$ are also discussed., Comment: 6 pages, 4 figures

We report an experimental study of the magnetic properties of infinite-layer Nd1-xSrxNiO2 thin films by x-ray magnetic circular dichroism (XMCD) at Ni L3,2 and Nd M5,4 edges. We show that at low temperatures the out-of-plane component of the Ni1+ spin-moment is characterized by a rapid increase for magnetic fields below 1T , followed by a slower linear increase reaching a spin-moment value of 0.25uB/Ni at 9T in the case of superconducting Nd0.8Sr0.2NiO2. On the other hand, the Nd M5,4 XMCD shows a clear paramagnetic behaviour, which make both Ni- and Nd-spin-sublattices fully uncorrelated.The magnetic field and temperature dependencies of the Ni L3,2 XMCD data can be explained by assuming an out-of-plane canting of the strongly in-plane anti-ferromagnetic ordered Ni1+ spins. A symmetry lowering of the NiO2 planes observed via four-dimensional scanning transmission electron microscopy, triggering a DMI, can be responsible of the proposed Ni1+ spin-canting at zero-field. The resulting out-of-plane weak-ferromagnetic coupling under magnetic field explains the relatively large spin-moment and its magnetic field and temperature dependence.

Infinite-layer nickelates $R_{1-x}$Sr$_{x}$NiO$_{2}$ ($R$ = La, Pr, Nd) are a class of superconductors with structural similarities to cuprates. Although long-range antiferromagnetic order has not been observed for these materials, magnetic effects such as antiferromagnetic spin fluctuations and spin-glass behavior have been reported. Different experiments have drawn different conclusions about whether the pairing symmetry is $s$- or $d$ wave. In this paper, we applied a scanning superconducting quantum interference device (SQUID) to probe the magnetic behavior of film samples of three infinite-layer nickelates (La$_{0.85}$Sr$_{0.15}$NiO$_2$, Pr$_{0.8}$Sr$_{0.2}$NiO$_2$, and Nd$_{0.775}$Sr$_{0.225}$NiO$_2$) grown on SrTiO$_3$ (STO), each with a nominal thickness of 20 unit cells. In all three films, we observed a ferromagnetic background. We also measured the magnetic susceptibility above the superconducting critical temperature in Pr$_{0.8}$Sr$_{0.2}$NiO$_2$ and La$_{0.85}$Sr$_{0.15}$NiO$_2$ and identified a non-Curie-Weiss dynamic susceptibility. Both magnetic features are likely due to NiO$_x$ nanoparticles. Additionally, we investigated superconductivity in Pr$_{0.8}$Sr$_{0.2}$NiO$_2$ and Nd$_{0.775}$Sr$_{0.225}$NiO$_2$, which exhibited inhomogeneous diamagnetic screening. The superfluid density inferred from the diamagnetic susceptibility in relatively homogeneous regions shows $T$-linear behavior in both samples. Finally, we observed superconducting vortices in Nd$_{0.775}$Sr$_{0.225}$NiO$_2$. We determined a Pearl length of 330 $\upmu$m for Nd$_{0.775}$Sr$_{0.225}$NiO$_2$ at 300 mK both from the strength of the diamagnetism and from the size and shape of the vortices. These results highlight the importance of considering NiO$_x$ particles when interpreting experimental results for these films.

We conducted a comparative study of the rare-earth infinite-layer nickelates films, RNiO2 (R = La, Pr, and Nd) using resonant inelastic X-ray scattering (RIXS). We found that the gross features of the orbital configurations are essentially the same, with minor variations in the detailed hybridization. For low-energy excitations, we unambiguously confirm the presence of damped magnetic excitations in all three compounds. By fitting to a linear spin-wave theory, comparable spin exchange coupling strengths and damping coefficients are extracted, indicating a universal magnetic structure in the infinite-layer nickelates. Interestingly, while signatures of a charge order are observed in LaNiO2 in the quasi-elastic region of the RIXS spectrum, it is absent in NdNiO2 and PrNiO2. This prompts further investigation into the universality and the origins of charge order within the infinite-layer inickelates., Comment: 8 figures. Accepted by Physical Review B

We report a $^{139}$La-NMR study of polycrystalline samples of multi($n$)-layered nickelates, La$_3$Ni$_2$O$_{7-\delta}$ ($n=2$) and La$_4$Ni$_3$O$_{10-\delta}$ ($n=3$), at ambient pressure. Measurements of the nuclear magnetic resonance (NMR) spectra and nuclear spin relaxation rate ($1/T_1$) indicate the emergence of a density wave order with a gap below $T^*\sim150$ K for La$_3$Ni$_2$O$_{7-\delta}$ and $\sim130$ K for La$_4$Ni$_3$O$_{10-\delta}$. The finite value of $1/T_1$ below $T^*$ indicates metallic ground states with the remaining density of states at the Fermi level ($E_{\rm F}$) under the density wave order. These features are attributed to multiple $d$ electron bands with different characteristics. Above $T^*$, the gradual decrease in $1/T_1T$ upon cooling implies the presence of a band with flat dispersion near $E_{\rm F}$. From our microscopic probes, we point out that these nickelates ($n=2$ and $3$) possess similar electronic states despite the difference in the formal valence of the Ni-$d$ electron states, which provides a basis for understanding the novel high-$T_{\rm c}$ superconductivity under high pressures., Comment: 5+1 pages, 3+1 figures

Infinite-layer nickelates show high-temperature superconductivity, and the experimental phase diagram agrees well with the one simulated within the dynamical vertex approximation (D$\Gamma$A). Here, we compare the spin-fluctuation spectrum behind these calculations to resonant inelastic X-ray scattering experiments. The overall agreement is good. This independent cross-validation of the strength of spin fluctuations strongly supports the scenario, advanced by D$\Gamma$A, that spin-fluctuations are the mediator of the superconductivity observed in nickelates., Comment: 13 pages, 8 figures

We report scanning tunnelling microscopy (STM) and x-ray photoemission spectroscopy (XPS) measurements on uncapped and SrTiO3 (STO) capped NdNiO2 realized by pulsed-laser deposition and topotactic reduction process. We find that untreated NdNiO2 surfaces are insulating and contain Ni mostly in a nominal Ni2+ oxidation state. Room temperature STM shows signatures of a striped-like topographic pattern, possibly compatible with recent reports of ordered oxygen vacancies in uncapped nickelates due to incomplete oxygen de-intercalation of the upper layers. A metallic surface and a full Ni1+ oxidation state is recovered by ultra high vacuum annealing at 250 C, as shown by STM and XPS. STO-capped NdNiO2 films, on the other hand, show Ni mostly in Ni1+ configuration, but Nd 3d5/2 core level spectra have a relevant contribution from ligand 4f 4L states, suggesting the formation of a NdTiNiOx layer at the interface with the STO. By in situ unit-cell by unit-cell Ar-ion sputtering removal of the STO capping and of the non stoichiometric interface layer, we were able to address the surface electronic properties of these samples, as shown by high resolution valence band photoemission spectroscopy. The results provide insights in the properties of infinite-layer NdNiO2 thin films prepared by the CaH2 topotactic reduction of perovskite NdNiO3 and suggest methods to improve their surface quality.