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Register a new userTopotactic hydrogen in nickelate superconductors and akin infinite-layer oxides ABO2
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Superconducting nickelates appear to be difficult to synthesize. Since the chemical reduction of ABO3 (A: rare earth; B transition metal) with CaH2 may result in both, ABO2 and ABO2H, we calculate the topotactic H binding energy by density functional theory (DFT). We find intercalating H is energetically favorable for LaNiO2 but not for Sr-doped NdNiO2. This has dramatic consequences for the electronic structure as determined by DFT+dynamical mean field theory: that of 3d9 LaNiO2 is similar to (doped) cuprates, 3d8 LaNiO2H is a two-orbital Mott insulator. Topotactical H might hence explain why some nickelates are superconducting and others are not.
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Two-level system (TLS) defects in dielectrics are known to limit the performance of electronic devices. We study TLS using millikelvin microwave loss measurements of three atomic layer deposited (ALD) oxide films--crystalline BeO ($rm{c-BeO}$), amorphous $rm{Al_2O_3}$ ($rm{a-Al_2O_3}$), and amorphous $rm{LaAlO_3}$ ($rm{a-LaAlO_3}$)--and interpret them with room temperature characterization measurements. We find that the bulk loss tangent in the crystalline film is 6 times higher than in the amorphous films. In addition, its power saturation agrees with an amorphous distribution of TLS. Through a comparison of loss tangent data to secondary ion mass spectrometry (SIMS) impurity analysis we find that the dominant loss in all film types is consistent with hydrogen-based TLS. In the amorphous films excess hydrogen is found at the ambient-exposed surface, and we extract the associated hydrogen-based surface loss tangent. Data from films with a factor of 40 difference in carbon impurities revealed that carbon is currently a negligible contributor to TLS loss.
The recent discovery of superconductivity in Nd$_{1-x}$Sr$_{x}$NiO$_2$ has drawn significant attention in the field. A key open question regards the evolution of the electronic structure with respect to hole doping. Here, we exploit x-ray absorption spectroscopy (XAS) and resonant inelastic x-ray scattering (RIXS) to probe the doping dependent electronic structure of the NiO$_2$ planes. Upon doping, a higher energy feature in Ni $L_3$ edge XAS develops in addition to the main absorption peak. By comparing our data to atomic multiplet calculations including $D_{4h}$ crystal field, the doping induced feature is consistent with a $d^8$ spin singlet state, in which doped holes reside in the $d_{x^2-y^2}$ orbitals, similar to doped single band Hubbard models. This is further supported by orbital excitations observed in RIXS spectra, which soften upon doping, corroborating with Fermi level shift associated with increasing holes in the $d_{x^2-y^2}$ orbital.
Recent scanning tunneling microscopy (STM) observation of U-shaped and V-shaped spectra (and their mixture) in superconducting Nd$_{1-x}$Sr$_x$NiO$_2$ thin films has been interpreted as presence of two distinct gap symmetries in this nickelate superconductor [Gu et al., Nat. Comm. 11, 6027 (2020)]. Here, using a two-band model of nickelates capturing dominant contributions from Ni-$3d_{x^2-y^2}$ and rare-earth (R)-$5d_{3z^2 - r^2}$ orbitals, we show that the experimental observation can be simply explained within a pairing scenario characterized by a conventional $d_{x^2-y^2}$-wave gap structure with lowest harmonic on the Ni-band and a $d_{x^2-y^2}$-wave gap with higher-harmonics on the R-band. We perform realistic simulations of STM spectra employing first-principles Wannier functions to properly account for the tunneling processes and obtain V, U, and mixed spectral line-shapes depending on the position of the STM tip within the unit cell. The V- and U-shaped spectra are contributed from Ni and R-bands, respectively, and Wannier functions, in essence, provide position-dependent weighing factors, determining the spectral line-shape at a given intra-unit cell position. We propose a phase-sensitive experiment to distinguish between the proposed $d$-wave gap structure and time-reversal symmetry breaking $d+is$ gap which yields very similar intra-unit cell spectra.
The electronic and magnetic properties of the new hydride superconductor CaFeAsH, which superconducts up to 47 K when electron-doped with La, and the isovalent alloy system CaFeAsH$_{1-x}$F$_x$ are investigated using density functional based methods. The $vec Q = (pi,pi,0)$ peak of the nesting function $xi(vec q)$ is found to be extremely strong and sharp, and additional structure in $xi(vec q)$ associated with the near-circular Fermi surfaces (FSs) that may impact low energy excitations is quantified. The unusual band introduced by H, which shows strong dispersion perpendicular to the FeAs layers, is shown to be connected to a peculiar van Hove singularity just below the Fermi level. This band provides a three dimensional electron ellipsoid Fermi surface not present in other Fe-based superconducting materials nor in CaFeAsF. Electron doping by 25% La or Co has minor affect on this ellipsoid Fermi surface, but suppresses FS nesting strongly, consistent with the viewpoint that eliminating strong nesting and the associated magnetic order allows high T$_c$ superconductivity to emerge. Various aspects of the isovalent alloy system CaFeAsH$_{1-x}$F$_x$ and means of electron doping are discussed in terms of influence of incipient bands.
A variety of nickel oxide compounds have long been studied for their manifestation of various correlated electron phenomena. Recently, superconductivity was observed in nanoscale infinite layer nickelate thin films of Nd$_{0.8}$Sr$_{0.2}$NiO$_2$, epitaxially stabilized on SrTiO$_3$ substrates via topotactic reduction from the perovskite precursor phase. Here we present the synthesis and properties of PrNiO$_2$ thin films on SrTiO$_3$. Upon doping in Pr$_{0.8}$Sr$_{0.2}$NiO$_2$, we observe superconductivity with a transition temperature of 7-12 K, and robust critical current density at 2 K of 334 kA/cm$^2$. These findings indicate that superconductivity in the infinite layer nickelates is relatively insensitive to the details of the rare earth 4$f$ configuration. Furthermore, they motivate the exploration of a broader family of compounds based on two-dimensional NiO$_2$ planes, which will enable systematic investigation of the superconducting and normal state properties and their underlying mechanisms.
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