Topotactic-hydrogen forms chains in $AB$O${}_2$ nickelate superconductors

Abstract

Despite enormous experimental and theoretical efforts, obtaining generally accepted conclusions regarding the intrinsic magnetic and electronic properties of superconducting nickelates remains exceptionally challenging. Experiments show a significant degree of uncertainty, indicating hidden factors in the synthesized films, which call for further investigations. One of those "hidden factors" is the possibility of intercalating hydrogen during the chemical reduction process from Nd(La)NiO${}_3$ to Nd(La)NiO${}_2$ using CaH${}_2$. While hydrogen has been detected in experimental samples, not much is known about its distribution through the crystal and its influence on the electronic environment. Here, we show the tendency toward the formation of one-dimensional hydrogen chains in infinite-layers LaNiO${}_2$ superconductors using density-functional theory (DFT) supplemented by dynamical mean-field theory (DMFT). The formation of such hydrogen chains induces a coexistence of different oxidation states of Ni and competing magnetic phases, and possibly explains the recently observed charge order states in nickelate superconductors. Furthermore, it contributes to the difficulty of synthesizing homogeneous nickelates and determining their ground states. The smoking gun to detect excess hydrogen in nickelates are flat phonon modes, which are infrared active and quite insensitive to the exact arrangement of the H atoms.

19 pages, 13 figures, under PRB review

References in corpus (54)

• Restoring the density-gradient expansion for exchange in solids and surfaces
• Generalized gradient approximation for solids and their surfaces
• Continuous-time Monte Carlo methods for quantum impurity models
• Novel Jeff = 1/2 Mott State Induced by Relativistic Spin-Orbit Coupling in Sr2IrO4
• Is LaO${}_{1-x}$F${}_x$FeAs an electron-phonon superconductor ?
• Dynamical vertex approximation - a step beyond dynamical mean field theory
• Orbital order and possible superconductivity in LaNiO3/LaMO3 superlattices
• Superconducting Dome in Nd${}_{1-x}$Sr${}_x$NiO${}_2$ Infinite Layer Films
• Phase diagram and superconducting dome of infinite-layer $\mathrm{N}{\mathrm{d}}_{1-\mathrm{x}}\mathrm{S}{\mathrm{r}}_{\mathrm{x}}\mathrm{Ni}{\mathrm{O}}_2$ thin films
• Superconductivity in a quintuple-layer square-planar nickelate
• Nickelate superconductivity without rare-earth magnetism: (La,Sr)NiO${}_2$
• Screened Coulomb interaction in the maximally localized Wannier basis
• Self-doped Mott insulator for parent compounds of nickelate superconductors
• Superconductivity in infinite-layer nickelate La${}_{1-x}$Ca${}_x$NiO${}_2$ thin films
• Late transition-metal oxides with infinite-layer structure: Nickelates versus cuprates
• Nickelate superconductors -- a renaissance of the one-band Hubbard model
• Phase Diagram of Infinite Layer Praseodymium Nickelate Pr${}_{1-x}$Sr${}_x$NiO${}_2$ Thin Films
• Doping evolution of the Mott-Hubbard landscape in infinite-layer nickelates
• Anomalous High-Energy Spin Excitations in La2CuO4
• Nickelate superconductors $--$ Multiorbital nature and spin freezing
• Charge density waves in infinite-layer NdNiO${}_2$ nickelates
• Role of $4f$ states in infinite-layer NdNiO${}_2$
• Charge and spin order dichotomy in NdNiO${}_2$ driven by SrTiO${}_3$ capping layer
• Intrinsic magnetism in superconducting infinite-layer nickelates
• Two-band model for magnetism and superconductivity in nickelates
• Orbital Selective Superconductivity in a Two-band Model of Infinite-Layer Nickelates
• Orbital and Spin Character of Doped Carriers in Infinite-Layer Nickelates
• Multiorbital processes rule the Nd${}_{1-x}$Sr${}_x$NiO${}_2$ normal state
• Conserved quantities of SU(2)-invariant interactions for correlated fermions and the advantages for quantum Monte Carlo simulations
• Materials design of dynamically stable $d^9$ layered nickelates
• Normal state of Nd${}_{1-x}$Sr${}_x$NiO${}_2$ from self-consistent $GW$+EDMFT
• Phase diagram of nickelate superconductors calculated by dynamical vertex approximation
• Fluctuation-frustrated flat band instabilities in NdNiO2
• Magnetic correlations in infinite-layer nickelates: an experimental and theoretical multi-method study
• NMR Evidence of Antiferromagnetic Spin Fluctuations in Nd${}_{0.85}$Sr${}_{0.15}$NiO${}_2$
• Electronic structure and magnetism in infinite-layer nickelates RNiO${}_2$ (R= La-Lu)
• Universal spin-glass behaviour in bulk LaNiO2, PrNiO2 and NdNiO2
• Superconductivity in Infinite-layer Nickelates : Role of Non-zero f-ness
• Bulk NdNiO2 is thermodynamically unstable with respect to decomposition while hydrogenation reduces the instability and transforms it from metal to insulator
• Antiferromagnetism in Ni-Based Superconductors
• Correlations turn electronic structure of finite-layer nickelates upside down
• Dynamical functional renormalization group computation of order parameters and critical temperatures in the two-dimensional Hubbard model
• Short-range magnetic interactions and spin-glass behavior in the quasi-2D nickelate Pr4Ni3O8
• Correlated interface electron gas in infinite-layer nickelate versus cuprate films on SrTiO${}_3$(001)
• Synthesis and physical properties of LaNiO${}_2$ crystals
• Magnetic properties and pseudogap formation in infinite-layer nickelates: insights from the single-band Hubbard model
• Geometric effects in the infinite-layer nickelates
• Investigation of hydrogen incorporations in bulk infinite-layer nickelates
• Cubic interaction parameters for t2g Wannier orbitals
• Correlated electronic structure of a quintuple-layer nickelate
• BaOsO${}_3$: A Hund's metal in the presence of strong spin-orbit coupling
• Signatures of topotactic hydrogen in nickelate superconductors
• Magnetism in doped infinite-layer NdNiO2 studied by combined density functional theory and dynamical mean-field theory
• Magnetic excitations in infinite-layer nickelates

Cited by in corpus (6)

• Correlated electronic structure, orbital-selective behavior, and magnetic correlations in double-layer La${}_3$Ni${}_2$O${}_7$ under pressure
• Closing in on possible scenarios for infinite-layer nickelates: comparison of dynamical mean-field theory with angular-resolved photoemission spectroscopy
• Topotactical Hydrogen Induced Single-Band $d$-wave Superconductivity in La${}_2$NiO${}_4$
• Lattice dynamics of the infinite-layer nickelate LaNiO${}_2$
• Theoretical study on the possibility of high $T_c$ s$\pm$-wave superconductivity in the heavily hole-doped infinite layer nickelates
• Discovery of Giant Unit-Cell Super-Structure in the Infinite-Layer Nickelate PrNiO${}_2$