arXiv subjects

Zihao Nie

Publications and source records attributed to Zihao Nie.

10 recordsLinked to original sources

arXiv2026

Electronic structures across superconductor-insulator transition in Ruddlesden-Popper bilayer nickelate films

High-transition-temperature ($T_{C}$) superconductivity is recently discovered in Ruddlesden-Popper (RP) nickelate films with extraordinarily strong oxidation. While investigating phase diagrams is essential for uncovering the superconducting mechanism, the oxygen-tuned superconductor-insulator transition (SIT) in RP nickelates differs fundamentally from that in cuprates or iron-based systems. Here, we unveil the evolution of electronic structure in RP bilayer nickelate thin films across the SIT, combining angle-resolved photoemission spectroscopy (ARPES) and X-ray absorption spectroscopy (XAS) for both occupied and unoccupied states. In the superconducting state, a coherent quasiparticle band near Fermi level ($E_{F}$) coexists with an incoherent waterfall feature at high energy, paralleling that in cuprates. Approaching the insulating state with oxygen deficiency, the spectral weight of the occupied coherent quasiparticle band is gradually suppressed, accompanied by pronounced density of states redistribution and orbital reconfiguration in unoccupied states. These results reveal the electronic origin of the SIT in the phase diagram, which transcends carrier doping effects and oxygen vacancy states. Our findings point to a decisive role of oxygen in shaping the essential electronic landscape of RP bilayer nickelates, offering crucial insights into the superconducting mechanism.

cond-mat.supr-con↗

arXiv2026

Superconductivity and Electronic Structures of Nickelate Thin Film Superstructures

Ruddlesden-Popper (RP) nickelates have emerged as a crucial platform for exploring the mechanisms of high-temperature superconductivity. However, the Fermi surface topology required for superconductivity remains elusive. Here, beyond the superconducting pure bilayer (2222) phase, we report the thin film growth and ambient-pressure superconductivity of monolayer-bilayer (1212) and bilayer-trilayer (2323) superstructures, together with the absence of superconductivity in monolayer-trilayer (1313) superstructure, under identical compressive epitaxial strain. The onset superconducting transition temperatures range from 46 to 50 K, exceeding the McMillan limit. Angle-resolved photoemission spectroscopy reveals key Fermi surface differences in these atomically-engineered structures. In superconducting 1212 and 2222 films, a dispersive hole-like band ($γ^{\mathrm{II}}$) forms an underlying Fermi pocket, surrounding the Brillouin zone corner. In contrast, the top of the flat band ($γ^{\mathrm{III}}$) is observed ~70 meV below $E_\text{F}$ in the non-superconducting 1313 films. Particularly, the superconducting 2323 films host both $γ^{\mathrm{II}}$ and $γ^{\mathrm{III}}$ bands. The polarization dependence of the $γ$ bands reveals their Ni $d_{z^2}$ origin. Our findings expand the family of ambient-pressure nickelate superconductors and establish a connection between structural configuration, electronic structure, and the emergence of superconductivity in nickelates.

cond-mat.supr-con↗

arXiv2026

Three-Dimensional Electronic Structures in Superconducting Ruddlesden-Popper Bilayer Nickelate Films

Beyond the quasi-two-dimensional (2D) paradigm of cuprates, the role of the third dimension of the Ruddlesden-Popper bilayer nickelates is essential to decoding their superconducting mechanism. Here, using angle-resolved photoemission spectroscopy (ARPES) with varied photon energies, we systematically investigate the electronic band structures in three dimensions for superconducting (La,Pr,Sm)$_3$Ni$_2$O$_7$/SrLaAlO$_4$ thin films (superconducting onset temperature $T_c^{\text{onset}} \sim 48$ K) transferred via a cryogenic ultra-high vacuum suitcase. We reveal an orbital-dependent dimensionality: while the $d{x^2-y^2}$-dominant bands exhibit a quasi-2D character, the $d{z^2}$-dominant band displays a finite $k_z$ dispersion. Finite energy gaps are identified on all observed bands across multiple high-symmetry directions. Systematic temperature-dependent analysis characterizes the superconducting nature of the gap on the $d{z^2}$-derived band, revealing a large gap $Δ\sim 18$ meV and a ratio $2Δ/k_BT_c\sim 8$ exceeding the weak-coupling BCS limit. The suppression of spectral weight near the Fermi level persists above the superconducting transition temperature. Ubiquitous waterfall-like spectral features evidence the presence of electron interactions. These results underscore the role of the $d_{z^2}$ orbital and correlations, placing constraints on theoretical models for nickelate superconductivity.

cond-mat.supr-con↗

arXiv2026

Superconductivity onset above 60 K in ambient-pressure nickelate films

Ambient-pressure superconductivity in nickelates has been capped at an onset transition temperature ($T_{c}^{onset}$) of ~50 K, a value that remains lower than the cuprate (~133 K) and iron-based (~55 K) counterparts, despite the promise shown under high pressure. Here, we report ambient-pressure superconductivity onset at ~63 K in epitaxial (La,Pr)3Ni2O7 thin films grown under compressive strain on SrLaAlO4 substrates. This $T_{c}$ leap is enabled by pushing our gigantic-oxidative atomic-layer-by-layer epitaxy (GAE) method into an extreme non-equilibrium growth regime. It simultaneously enhances kinetics via higher temperatures and achieves full oxygenation in situ without post-annealing. Synchrotron X-ray diffraction and scanning transmission electron microscopy confirm that this approach yields films of large-scale crystalline purity, overcoming the inherent metastability of the strained superconducting phase. Transport measurements reveal a zero-resistance temperature ($T_{c}^{zero}$) reaching ~37 K, while mutual inductance measurements demonstrate a robust diamagnetic transition starting at ~23 K. These films exhibit a systematic evolution in their normal-state resistivity-temperature curve: the power-law exponent $α$ evolves from Fermi-liquid-like ($α$ ~2) at lower $T_{c}^{onset}$ to strange-metal-like ($α$ ~1) in higher $T_{c}^{onset}$ samples, directly linking the enhanced superconductivity to non-Fermi liquid behavior. Mapping the vortex melting phase diagram by the mutual inductance technique further reveals 2D melting limit suppressed to near zero, which demonstrates significantly stronger interlayer coupling than that of cuprates. These results identify the nickelates as an ambient-pressure strange-metal high-temperature superconductors with strong interlayer coupling.

cond-mat.supr-con↗

arXiv2026

Preparation and optimization of high-temperature superconducting Ruddlesden-Popper nickelate thin films

The discovery of ambient-pressure nickelate high-temperature superconductivity provides a new platform for probing the underlying superconducting mechanisms. However, the thermodynamic metastability of Ruddlesden-Popper nickelates Lnn+1NinO3n+1 (Ln = lanthanide) presents significant challenges in achieving precise control over their structure and oxygen stoichiometry. This study establishes a systematic approach for growing phase-pure, high-quality Ln3Ni2O7 thin films on LaAlO3 and SrLaAlO4 substrates using gigantic-oxidative atomic-layer-by-layer epitaxy. The films grown under an ultrastrong oxidizing ozone atmosphere are superconducting without further post annealing. Specifically, the optimal Ln3Ni2O7/SrLaAlO4 superconducting film exhibits an onset transition temperature (Tc,onset) of 50 K. Four critical factors governing the crystalline quality and superconducting properties of Ln3Ni2O7 films are identified: 1) precise cation stoichiometric control suppresses secondary phase formation; 2) complete atomic layer-by-layer coverage coupled with 3) optimized interface reconstruction minimizes stacking faults; 4) accurate oxygen content regulation is essential for achieving a single superconducting transition and high Tc,onset. These findings provide valuable insights for the layer-by-layer epitaxy growth of diverse oxide high-temperature superconducting films.

cond-mat.supr-con↗

arXiv2026

Superconductor-insulator transitions in infinite-layer nickelates controlled via ${operando}$ monitored reduction

Nickelates represent an emerging class of superconductors that demand innovative approaches for structural and electronic phase modulations. Continuous control over superconductor-insulator transition (SIT) in nickelates remains particularly challenging, hindering both fundamental understanding and potential applications. Here, we demonstrate SIT in infinite-layer nickelate superconductors utilizing multiple techniques, including an ${operando}$ monitored reduction (OMR) method. OMR enables ultrawide-range continuous modulation of the Ni 3${d}$ orbital electron occupancy from ~3${d}^7$ to ~3${d}^9$. The 3${d}$ occupancy is calibrated through systematic synchrotron X-ray absorption (XAS), combined with scanning transmission electron microscopy (STEM) annular bright field (ABF) analysis of oxygen atoms. SIT is further modulated via ionic liquid gating and magnetic field. Strikingly different from cuprates, our Nernst effect measurements show that pairing initiates at the onset of the resistive drop. The subsequent emergence of the Meissner effect at zero resistance marks the establishment of global phase coherence. Angle-dependent magnetotransport within the transition temperature regime indicates a mixture of two-dimensional (2D) and three-dimensional (3D) superconducting characters, suggesting the observed SIT deviates from the canonical 2D model. Our results provide a unique perspective on the interplay of structural and electronic phase transitions in the infinite-layer nickelates across the oxygen content-magnetic field-temperature parameter space.

cond-mat.supr-con↗

arXiv2025

Nodeless superconducting gap and electron-boson coupling in (La,Pr,Sm)$_{3}$Ni$_2$O$_7$ films

The discovery of superconductivity in Ruddlesden-Popper (RP) bilayer nickelate films under ambient pressure provides an unprecedented opportunity to directly investigate electronic energy scales of the superconducting state and the pairing mechanism. Here, we report angle-resolved photoemission spectroscopy measurements of superconducting (La,Pr,Sm)$_{3}$Ni$_2$O$_7$ thin films epitaxially grown on SrLaAlO$_4$ substrates by developing an ultra-high vacuum low-temperature quenching and transfer technique. A finite superconducting gap of ~18 meV with pronounced coherence peak is observed along the Brillouin zone diagonal direction. Remarkably, the finite superconducting gap persists across the entire Brillouin zone of the underlying Fermi surfaces, revealing the absence of gap nodes. An abrupt band renormalization, manifested as a kink in the energy-momentum dispersion at ~70 meV below the Fermi level, indicates an electron-boson coupling in the system. The simultaneous observation of a nodeless superconducting gap and electron-boson coupling provides crucial insights into the pairing symmetry and gluing mechanism in high-T$_c$ RP bilayer nickelates.

cond-mat.supr-con↗

arXiv2025

Angle-resolved photoemission spectroscopy of superconducting (La,Pr)3Ni2O7/SrLaAlO4 heterostructures

Ruddlesden-Popper bilayer nickelate thin film superconductors discovered under ambient pressure enable vast possibilities for investigating electronic structures of the superconducting state. Here, we report angle-resolved photoemission spectroscopy (ARPES) measurements of 1, 2, and 3 unit-cell epitaxial La2.85Pr0.15Ni2O7 films grown on SrLaAlO4 substates, through pure-oxygen in situ sample transportation. Evidence obtained using photons with distinct probing depths shows that conduction is localized primarily at the first unit cell near the interface. Scanning transmission electron microscopy (STEM), together with energy-dispersive X-ray spectroscopy (EDS) and electron energy loss spectroscopy (EELS), indicates that interfacial Sr diffusion and pronounced p-d hybridization gradient may collectively account for the interfacial confinement of conduction. Fermi surface maps reveal hole doping compared to non-superconducting ambient-pressure bulk crystals. Measurements of dispersive band structures suggest the contributions from both Ni dx2-y2 and dz2 orbitals at the Fermi level. Density functional theory (DFT) + U calculations capture qualitative features of the ARPES results, consistent with a hole-doped scenario. These findings constrain theoretical models of the superconducting mechanism and suggest potential for enhancing superconductivity in nickelates under ambient pressure.

cond-mat.supr-con↗

arXiv2024

Ambient-pressure superconductivity onset above 40 K in bilayer nickelate ultrathin films

The discovery of bilayer nickelate superconductors under high pressure has opened a new chapter in high-transition temperature (high-TC) superconductivity. Here, we report ambient-pressure superconductivity onset above the McMillan limit (40 K) in bilayer nickelate epitaxial ultrathin films. Three-unit-cell (3UC) thick La2.85Pr0.15Ni2O7 single-phase-crystalline films are grown using the gigantic-oxidative atomic-layer-by-layer epitaxy (GOALL-Epitaxy) on SrLaAlO4 substrates. Resistivity measurements and magnetic-field responses indicate onset TC = 45 K. The transition to zero resistance exhibits characteristics consistent with a Berezinskii-Kosterlitz-Thouless (BKT)-like behavior, with TBKT = 9 K. Meissner diamagnetic effect is observed at TM = 8.5 K via a mutual inductance setup, in agreement with the BKT-like transition. In-plane and out-of-plane critical magnetic fields exhibit anisotropy. Scanning transmission electron microscopy (STEM) images and X-ray reciprocal space mappings (RSMs) show that the films maintain a tetragonal phase with coherent epitaxial compressive strain ~2% in the NiO2 planes relative to the bulk. Our findings pave the way for comprehensive investigations of nickelate superconductors under ambient pressure conditions and for exploring superconductivity at higher transition temperature through strain engineering in heterostructures.

cond-mat.supr-con↗

arXiv2024

Gigantic-oxidative atomic-layer-by-layer epitaxy for artificially designed complex oxides

In designing material functionalities for transition metal oxides, lattice structure and d-orbital occupancy are key determinants. However, the modulation of these two factors is inherently limited by the need to balance thermodynamic stability, growth kinetics, and stoichiometry precision, particularly for metastable phases. We introduce a methodology, namely the gigantic-oxidative atomic-layer-by-layer epitaxy (GOALL-Epitaxy), enhancing oxidation power 3-4 orders of magnitude beyond conventional pulsed laser deposition (PLD) and oxide molecular beam epitaxy (OMBE), while ensuring atomic-layer-by-layer growth of designed complex structures. Thermodynamic stability is markedly augmented with stronger oxidation at elevated temperatures, whereas growth kinetics is sustained by laser ablation at lower temperatures. We demonstrate the accurate growth of complex nickelates and cuprates, especially an artificially designed structure with alternating single and double NiO2 layers possessing distinct nominal d-orbital occupancy, as a parent of high-temperature superconductor. The GOALL-Epitaxy enables material discovery within the vastly broadened growth parameter space.

cond-mat.str-el↗