The discovery of high-temperature ferromagnetism in the metallic van der Waals (vdW) system Fe_NGeTe_2 has brought two-dimensional (2D) magnets into technologically relevant temperature scales. Specifically at N = 5, dilution of magnetic moments by nickel substitution counterintuitively achieves a record high Curie temperature of 478 K. Unraveling the origin of this nickel-substitution-induced enhancement is complicated by the compound's structural complexity, coexistent itinerant and local magnetic contributions, and mesoscopic compositional domains. Through coordinated structural and electronic characterization, we identify that the high-T_C magnetic phase arises from a strain-stabilized Fe_6GeTe_2 nano-precipitate. Combining first-principles calculations and spin- and angle-resolved photoemission spectroscopy (ARPES), we uncover a site-specific electronic landscape in which interior iron atoms primarily host localized moments while the outer iron atoms neighboring the tellurium layers produce spin-polarized itinerant carriers that cross the vdW gap. The large energy cost associated with homogeneous nickel substitution is found to favor the spontaneous precipitation of the crystallographically and electronically “clean” high-T_C phase. Finally, we compare metal-rich vdW magnets with binary magnetic alloys, and discuss the unifying roles of nano-precipitates in stabilizing otherwise unattainable bulk phases. Our work provides mechanistic insights into the record-high T_C ferromagnetism in (Fe,Ni)_5+δGeTe_2, establishing a rigorous foundation for the atomic engineering of vdW magnetic metals informed by direct electronic signatures.

Decoherence remains a critical obstacle to achieving high-fidelity, scalable superconducting qubits, with the tunnel barrier of Josephson junctions a key source of loss. Here we apply resonant X-ray reflectivity to non-destructively probe the electronic structure of buried layers in Al/AlO_x/Al Josephson junctions. At the Al K-edge, energy-dependent modulations in the reflectivity maps enable Kramers-Kronig-constrained extraction of the layer-resolved atomic scattering factors. The analysis reveals that the barrier coordination evolves from more tetrahedral toward predominantly octahedral character with increasing oxidation pressure. At the interfaces, the lower metal-oxide boundary is comparatively under-coordinated and disordered relative to the upper interface. Comparison with simulated X-ray absorption spectra identifies the dominant coordination motifs within the oxide and its interfaces, providing depth-resolved structural insight that constrains microscopic models of two-level system formation. These results link growth conditions, local coordination environments, and junction electronic properties, demonstrating resonant X-ray reflectivity as a powerful tool for probing the microscopic materials properties of Josephson junctions and providing a materials-level framework for mitigating decoherence in superconducting qubits.

The discovery of superconductivity in bulk bilayer nickelates under high pressure, and its subsequent stabilization in compressively strained thin films at ambient pressure, has established a new platform for exploring high-T_{c} superconductivity beyond the cuprates. Central to this development is the prominent role of the 3d_{z}^{2} orbital in shaping the low-energy electronic structure, imposing constraints on microscopic theories and fueling debate over the superconducting mechanism. Here we report a systematic in situ angle-resolved photoemission spectroscopy study of compressively strained bilayer nickelate thin films spanning Ca doping, oxygen stoichiometry and film thickness. Despite variations in oxygen-vacancy disorder and surface termination, the electronic structure remains robust and exhibits a systematic strain-driven evolution consistent with an intermediate-correlation regime. In particular, we demonstrate a Ca-doping-induced electronic structure evolution that is consistent with Fermi-level crossing of the γ band and is decoupled from the presence of superconductivity, suggesting that, while important for the γ band to be near the Fermi level, the debated γ crossing and the resulting Fermi pocket may not be a prerequisite for superconductivity. Together, our results establish key spectroscopic constraints on the minimal fermiology and correlation strength relevant to superconductivity in bilayer nickelates, providing an experimental foundation for microscopic theories of their pairing mechanism.

Abstract In multilayered high- T c cuprates, the inner CuO 2 planes (IPs) are spatially separated from dopant layers and thus remain cleaner than the outer planes (OPs). Here, we investigate five-layer (Cu,C)Ba 2 Ca 4 Cu 5 O y (Cu1245) and three-layer Ba 2 Ca 2 Cu 3 O 6 (F,O) 2 (F0223) using angle-resolved photoemission spectroscopy (ARPES) and uncover an unprecedented situation, in which only the IPs become superconducting while the OPs remain metallic at low temperatures. Our model calculations indicate that over 95% of the OP wavefunction remains confined to OP itself, rendering superconducting proximity negligible. This interlayer decoupling realizes an ideal configuration—a single superconducting CuO 2 layer screened from the dopant layer-induced disorder by heavily overdoped metallic OPs. The clean CuO 2 layer exhibits a large superconducting gap with coherent Bogoliubov peaks extending beyond the antiferromagnetic zone boundary, and a widely extended coherent flat band at the Brillouin zone edge. These findings introduce the “degree of screening” as a physical parameter for probing competition between pseudogap and superconductivity, and for bridging typically disordered real materials with the idealized theoretical models.

Abstract Fermi arcs observed in underdoped cuprates have sparked debate over whether they represent segments of a large Fermi surface or small Fermi pockets. This ambiguity has long hindered their classification as either the conventional Bardeen-Cooper-Schrieffer (BCS) regime or the strongly coupled Bose-Einstein condensation (BEC) crossover limit. Here, using angle-resolved photoemission spectroscopy and quantum oscillations, we demonstrate the coexistence of a small Fermi pocket and a large superconducting gap in the clean inner CuO2 layers of the four-layer cuprate Ba2Ca3Cu4O8(F,O)2. This coexistence constitutes a hallmark of the BCS-BEC crossover and has remained elusive for decades. Despite the presence of antiferromagnetic (AF) order, the superconducting gap in the small pocket is remarkably large, yielding a gap-to-Fermi energy ratio (Δpocket/ε F ~ 0.6) and a critical-to-Fermi temperature ratio (T c/T F ~ 0.13) that reach the theoretical upper bound for two-dimensional superconductivity. Unexpectedly, this BCS-BEC crossover emerges not as the carrier density decreases but as it increases, abruptly within a narrow doping range of less than 1%. These results provide a long-sought microscopic foundation for the d-wave pairing mechanism in doped AF-Mott insulators.

Understanding how strong electronic correlations shape superconductivity remains a central challenge in quantum materials. In multiorbital systems, correlations driven by Hund's coupling can differentiate the behavior of individual orbitals, producing the so-called Hund's metal state. How such orbital-selectivity also governs superconducting pairing, however, has remained largely unexplored experimentally. Here we use high-resolution angle-resolved photoemission spectroscopy to systematically map the superconducting gap structure across the phase diagram of the representative iron-based superconductor Ba1-xKxFe2As2. We find that superconductivity evolves in a strongly orbital-dependent manner: the gap associated with the dxy orbital collapses beyond optimal doping while pairing on the dxz/dyz orbitals persists. This behavior mirrors the orbital-selective correlations observed in the normal state and reveals a direct connection between Hund's metal physics and the superconducting pairing landscape. Our results demonstrate that superconducting gaps themselves can serve as a sensitive probe of orbital-dependent correlations and suggest that Hund's coupling plays a central role in shaping pairing in multiorbital superconductors.

Combining topological insulators with topological semimetals in the form of homologous superlattices is a promising approach for generating correlated quantum matter based upon Fermi level alignment with band extrema. For antimony telluride, a saddle point is predicted to occur at the M-point, while antimonene layering is predicted to move the M-point valence band towards the Fermi level. To date, the predicted saddle point at the M-point has not yet been demonstrated, and studies of antimony telluride homologous superlattices have been limited to one or two layers of antimonene added to antimony telluride. Here, we present scanning tunneling spectroscopy and angle-resolved photoemission spectroscopy studies of a series of antimony telluride homologous superlattices with two to four layers of antimonene. In addition to demonstrating the presence of a saddle point and associated van Hove singularity near the M-point, we identify the key role of Sb and Te p_z orbital hybridization in driving the van Hove singularity toward the Fermi level.

The interplay among orbital-selective Mott physics, Hund's coupling, tunable structural motifs, and Kondo-like scattering establishes a compelling paradigm for understanding and engineering correlated multi-orbital systems, as vividly exemplified by nickelate superconductors. Here, using high-resolution angle-resolved photoemission spectroscopy combined with theoretical calculations, we systematically investigate the electronic properties of trilayer nickelates. In La4Ni3O10, we observe pronounced interorbital hybridization, whereas in Pr4Ni3O10, the flat d_(z^2 ) band becomes markedly incoherent and diminishes in spectral weight. By contrast, the dispersive d_(x^2-y^2 ) bands retain coherence in both compounds. This striking incoherence/coherence dichotomy identifies an orbital-selective Mott phase modulated by the interlayer Ni-O-Ni bonding angle. The depletion of the d_(z^2 ) orbitals further frustrates the interorbital hybridization and influences the density-wave transition in Pr4Ni3O10. Moreover, the density-wave gap is substantially reduced in Pr4Ni3O10, likely due to extra scattering channels provided by the local moments of Pr3+ cations. Our findings elucidate the intricate interplay among lattice, orbital, spin, and electronic degrees of freedom and reveal a feasible structural control parameter for the multi-orbital correlated state in trilayer nickelates, which provide a concrete framework for understanding the emergence of superconductivity under high pressure.

Among the family of intercalated transition-metal dichalcogenides (TMDs), Fe_xNbS_2 is found to possess unique current-induced resistive switching behaviors, tunable antiferromagnetic states, and a commensurate charge order, all of which are tied to a critical Fe doping of x_c = 1/3. However, the electronic origin of such extreme stoichiometry sensitivities remains unclear. Combining angle-resolved photoemission spectroscopy (ARPES) with density functional theory (DFT) calculations, we identify and characterize a dramatic eV-scale electronic restructuring that occurs across the x_c. Moment-carrying Fe 3d_z^2 electrons manifest as narrow bands within 200 meV of the Fermi level, distinct from other transition metal intercalated TMD magnets. These states strongly hybridize with itinerant electrons in TMD layer, rapidly lose coherence above x_c due to correlation-driven effects. This sudden quasiparticle decoherence collapses the Fe-Nb hybridization, which explicitly suppresses the out-of-plane effective Fe-Fe exchange interaction, driving the transformation of the magnetic ground state from an antiferromagnetic stripe phase to a zigzag phase. These observations resemble the exceptional electronic and magnetic sensitivity of strongly correlated systems, and demonstrate that quantifying orbital-specific hybridization via ARPES offers an alternative pathway to evaluate effective magnetic exchange in metallic magnets, complementing inelastic neutron and resonant x-ray scattering probes.

Charge density waves (CDWs) offer versatile platforms for accessing metastable states due to their sensitivity to external stimuli. However, most metastable CDW states are stabilized only at low temperatures, limiting their practical utility. In this study, we report the observation of electrically driven, room-temperature, nonvolatile metastable states in the bulk form of EuTe4, a recently discovered compound that hosts an innate moiré superlattice characterized by the stacking of incommensurate monolayer and bilayer CDWs. Systematic transport measurements reveal discrete resistivity plateaus and strong electric-field sensitivity, with a large number of metastable states readily induced across a wide temperature window within a giant hysteresis loop, making them well-suited for high-temperature, multi-bit memory applications. By integrating photoemission spectroscopy, diffraction, and in-situ transport measurements, we uncover that these metastable states are characterized by a suppression of the original CDW amplitude and a reduction in correlation length, pointing to a unique electric-field-induced switching of out-of-plane CDW phases in the moiré superstructure. Our findings provide critical insights into metastable phenomena in moiré systems with stacked electronic orders and establish EuTe4 as a promising platform for developing room-temperature, multi-bit memory devices.

Quantum materials with bands of narrow bandwidth near the Fermi level represent a promising platform for exploring a diverse range of fascinating physical phenomena, as the high density of states within the small energy window often enables the emergence of many-body physics. On one hand, flat bands can arise from strong Coulomb interactions that localize atomic orbitals. On the other hand, quantum destructive interference can quench the electronic kinetic energy. Although both have a narrow bandwidth, the two types of flat bands should exhibit very distinct spectral properties arising from their distinctive origins. So far, the two types of flat bands have only been realized in very different material settings and chemical environments, preventing a direct comparison. Here we report the observation of the two types of flat bands within the same material system-an above-room-temperature van der Waals ferromagnet, Fe5-xGeTe2, distinguishable by a switchable iron site order. The contrasting nature of the flat bands is also identified by the remarkably distinctive temperature evolution of the spectral features, indicating that one arises from electron correlations in the Fe(1) site-disordered phase, while the other geometrical frustration in the Fe(1) site-ordered phase. Our results therefore provide a direct juxtaposition of the distinct formation mechanism of flat bands in quantum materials and an avenue for understanding the distinctive roles flat bands play in the presence of magnetism, topology, and lattice geometrical frustration, utilizing sublattice ordering as a key control parameter.

The mechanism behind superconductivity suppression induced by Pr substitutions in YBa2Cu3O7-δ (YBCO) has been a mystery since its discovery: in spite of being isovalent to Y3+ with a small magnetic moment, it is the only rare-earth element that has a dramatic impact on YBCO's superconducting properties. Using angle-resolved photoemission spectroscopy (ARPES) and DFT+[Formula: see text] calculations, we uncover how Pr substitution modifies the low-energy electronic structure of YBCO. Contrary to the prevailing Fehrenbacher-Rice (FR) and Liechtenstein-Mazin (LM) models, the low-energy electronic structure contains no signature of any f-electron hybridization or additional f-state Fermi surface sheets. Yet, strong electron doping is observed primarily on the antibonding Fermi surface. Meanwhile, we reveal major electronic structure modifications to Cu-derived states with increasing Pr substitution: a pronounced CuO2 bilayer decoupling and enhanced hopping along the CuO chain, implying indirect electron-release pathways beyond simple 4f state ionization. Our results challenge the long-standing FR/LM mechanism, and establish Pr substituted YBCO as a potential platform for exploring correlation-driven phenomena in coupled 1D-2D systems.

Metastability is fundamental not only to phase ordering and transitions, but also to a broad range of modern technologies, from memory devices to metallic glasses. In condensed-matter physics, charge density waves (CDWs) offer versatile platforms for accessing metastable states due to their sensitivity to external stimuli. However, most metastable CDW states are stabilized only at low temperatures, limiting their practical utility. In this study, we report the observation of electrically driven, room-temperature, nonvolatile metastable states in the bulk form of EuTe_4, a recently discovered compound that hosts an innate moiré superlattice characterized by the stacking of incommensurate monolayer and bilayer CDWs. Systematic transport measurements reveal discrete resistivity plateaus and strong electric-field sensitivity, with a large number of metastable states readily induced across a wide temperature window within a giant hysteresis loop, making them well-suited for high-temperature, multi-bit memory applications. By integrating photoemission spectroscopy, diffraction, and in-situ transport measurements, we uncover that these metastable states do not stem from conventional mechanisms such as the emergence of new ordered phases or changes in incommensurate periodicity. Instead, they are characterized by a suppression of the original CDW amplitude and a reduction in correlation length, pointing to a unique electric-field-induced switching of out-of-plane CDW phases in the moiré superstructure. Our findings not only provide critical insights into metastable phenomena in moiré systems with stacked electronic orders but also establish EuTe_4 as a promising platform for developing room-temperature, multi-bit memory devices.

As strong topological insulators, Bi1-xSbxalloys with∼0.07<x<0.22are predicted to host topologically protected conduction pathways along extended defects, such as dislocations. Due to the presence of bulk conduction, these fascinating topological features have been obscured to date. We examine carrier transport and electronic states in high-purity single-crystals of Bi1-xSbxalloys with 11 at% Sb. Using high magnetic fields, we suppress bulk conduction, enabling the identification of the residual conductivity associated with extended defects. A two-band analysis of magnetotransport measurements in combination with angle-resolved photoemission spectroscopy, reveals a bandgap⩾40 meV, larger than Arrhenius analyses of temperature-dependent resistivities. With mobility as high as 750 000 cm2 V-1 s-1, Bi-Sb alloys are promising candidates for topological electronics and related applications.

While the superconducting transition temperature of hole-doped Ba_{1-x}K_{x}Fe_{2}As_{2} decreases past optimal doping, superconductivity does not completely disappear even for the fully doped KFe_{2}As_{2} compound. In fact, superconductivity is robust through a Lifshitz transition where electron bands become hole-like around the zone corner at around x=0.7, thus challenging the conventional understanding of superconductivity in iron-based systems. High-resolution angle-resolved photoemission spectroscopy is used to investigate the superconducting gap structure, as well as the normal state electronic structure, around optimal doping and across the Lifshitz transition. Our findings reveal a largely orbital-dependent superconducting gap structure, where the more strongly correlated d_{xy} band has a vanishing superconducting gap at higher doping, aligning with the Hund's metal behavior observed in the normal state. Notably, the superconducting gap on the d_{xy} band disappears before the Lifshitz transition, suggesting that the Fermi surface topology may play a secondary role. We discuss how these results point to orbital-selective superconducting pairing and how strong correlations via Hund's coupling may shape superconducting gap structures in iron-based and other multiorbital superconductors.

Moiré superlattices, engineered through precise stacking of van der Waals (vdW) layers, hold immense promise for exploring strongly correlated and topological phenomena. However, these applications have been held back by the common preparation method: tear-and-stack of Scotch tape exfoliated monolayers, which suffer from low efficiency and reproducibility, twist angle inhomogeneity, interfacial contamination, and micrometer sizes. Here, we report an effective strategy to construct highly consistent mixed-dimensional and twisted bilayer vdW moiré structures with high production throughput, near-unity yield, pristine interfaces, precisely controlled twist angles, and macroscopic scale (up to centimeters) with enhanced thermal stability. We demonstrate the versatility across various vdW materials, including transition metal dichalcogenides, graphene, and hBN. The expansive size and high quality of moiré structures enable reciprocal-space high-resolution mapping of the superlattices and back-folded moiré mini band structures with low energy electron diffraction (LEED) and angle-resolved photoemission spectroscopy (ARPES). In particular, we identify the backfolded bands at the K point of twisted transition metal dichalcogenide moiré structures. This technique will have broad applications in both fundamental studies and the mass production of twistronic devices.

Intertwined orders appear when multiple orders are strongly interacting, and kagome metals have emerged as new platforms to explore exotic phases. FeGe has been found to develop a charge density wave (CDW) order within magnetic phase, suggesting an intricate interplay of the lattice, charge, and spin degrees of freedom. Recently, postgrowth annealing has been proposed to tune the CDW order from long-range to complete suppression, offering a tuning knob for the CDW order. Here, by comparing the electronic structures of FeGe subjected to different annealing conditions and distinct CDW properties, we report spectral evolution associated with the lattice and spin degrees of freedom. We find band evolution linked to a spin density wave (SDW) order present in both samples with and without CDW order, and another evolution connected to the lattice distortions that onset with the long-range CDW order and revert with the SDW order. Our results reveal a rare competitive cooperation of the lattice, spin, and charge in FeGe.

Non-Fermi liquid (non-FL) phase is a pivotal enigma in understanding intriguing quantum phases in strongly correlated systems, such as high-temperature superconductivity. Tomonaga-Luttinger liquid (TLL) theory, designed for one-dimensional (1D) systems, serves as one of the microscopic frameworks that elucidates non-FL behavior. Despite its theoretical concreteness, comprehensive experimental verification has remained incomplete. In particular, addressing the persistence of the TLL nature within ordered phases, such as charge density wave (CDW), has posed a significant challenge. We report the observation of TLL characteristics across the CDW transitions in a quasi-1D material NbSe_{3} using angle-resolved photoemission spectroscopy. Spin-charge separation, a disentanglement of spin and charge degrees of freedom of electrons, is clearly observed within the band, accompanied by the suppression of spectral weight following a power-law behavior with anticipated temperature scaling. Surprisingly, the spin-charge separation persists even below the CDW transition temperatures, indicating the validity of the TLL nature in the CDW phase. Our findings offer a unique opportunity to explore the interplay between the TLL and ordered phases, which could be connected to the interplay between non-FL and ordered phases in strongly correlated systems.