SrCu2(BO3)2 (SCBO) is a paradigmatic realization of the Shastry-Sutherland model, hosting geometrically frustrated spin dimers and a variety of quantum magnetic phases and phenomena. Although its magnetic properties have been extensively studied, the high-energy electronic excitations that determine the crystal-field environment and Cu-O hybridization have remained largely unexplored. Here we combine Cu L3-edge resonant inelastic x-ray scattering (RIXS), broadband optical spectroscopy, and electronic-structure calculations to determine the relevant local and interband excitation energy scales in SCBO. RIXS resolves a well-defined manifold of localized Cu2+ d-d excitations between 1.8 and 2.4 eV, whose energies and polarization dependence are well reproduced by multireference quantum-chemistry calculations. In contrast, optical spectroscopy identifies charge-transfer excitations with an absorption onset near 1.2-1.6 eV and a broader higher-energy structure around 4.5 eV, which are qualitatively captured by DFT+U calculations. Taken together, these results define the characteristic energy scales of d-d and CT excitations, offering quantitative benchmarks for computational frameworks and providing essential input for refining superexchange-based magnetic models of this prototypical frustrated quantum antiferromagnet.
The recent discovery of high-temperature superconductivity in hole-doped SmNiO2, exhibiting the record-high transition temperature Tc among infinite-layer (IL) nickelates, has opened a new avenue for exploring design principles of superconductivity. Experimentally determining the electronic structure and magnetic interactions in this new system is crucial to elucidating the mechanism behind the enhanced superconductivity. Here, we report a Ni L-edge resonant inelastic x-ray scattering (RIXS) study of superconducting Sm-based IL nickelate thin films Sm1-x-yEuxCayNiO2 (SECNO). Dispersive paramagnonic excitations are observed in both optimally and overdoped SECNO samples, supporting a spin-fluctuation-mediated pairing scenario. However, despite the two-fold enhancement of Tc in the Sm-based nickelates compared to their Pr-based counterparts, the effective exchange coupling strength is reduced by approximately 20%. This behavior contrasts with hole-doped cuprates, where magnetic interactions correlate positively with Tc, highlighting essential differences in their superconducting mechanisms.
A major challenge in condensed matter physics is integrating topological phenomena with correlated electron physics to leverage both types of states for next-generation quantum devices. Metal-insulator transitions are central to bridging these two domains while simultaneously serving as on-off switches for electronic states. Here, we demonstrate how the prototypical material of K2Cr8O16 undergoes a ferromagnetic metal-insulator transition accompanied by a change in band topology. Through inelastic x-ray and neutron scattering experiments combined with first-principles theoretical calculations, we show that this transition is not driven by a Peierls mechanism, given the lack of phonon softening. Instead, we establish the transition as a topological metal-insulator transition within the ferromagnetic phase with potential axionic properties, where electron correlations play a key role in stabilizing the insulating state. These results reveal how a metal-insulator transition provides a pathway through which magnetism, topology, and electronic correlations interact.
Solid matter is classified through symmetry of ordering phenomena. Experimentally, this approach is straightforward, except when distinct orderings occur with identical or almost identical symmetry breaking. Here we show that the cuprate system Y1-xPrxBa2Cu3O6+y hosts two distinct orderings with almost identical translational symmetry breaking. Only when applying site-sensitive resonant elastic x-ray scattering, charge ordering can be conclusively differentiated from a super-lattice structure. These two orderings manifest at different atomic sites and display different temperature dependence. Differentiating these orders provides an important clue to the anomalous behavior of PrBa2Cu3O7 within the 123-series of high-temperature superconductors. The superstructure symmetry breaking at the Pr-site should be included into future models of the unusual insulating ground state of PrBa2Cu3O7.
Superconductivity in cuprates emerges out of a complex normal state that hosts density waves, pseudogap physics, and strange metal properties. Here, we access this normal state by synchronizing free-electron laser x-rays with high-magnetic-field pulses up to 44 T. We observe a linear increase in charge order amplitude and correlation length that persists far above the vortex melting transition. This behavior is incompatible with standard phase competition between charge order and superconductivity. By means of conventional hard x-ray diffraction and magnetostriction, we show that applied fields also enhance monoclinic lattice distortions. However, this magnetoelastic response is weaker and an epiphenomenon of the stripe order enhancement. Combined with recent observations of field-linear spin freezing, our results point to a direct coupling between magnetic field and the spin component of stripe order in the high-field normal state – a mechanism independent of superconductivity suppression that has so far remained hidden from scattering probes.
Side surfaces of cuprate superconductors are expected to display a suppressed d-wave order parameter and zero-energy topological flat bands with a large density of states, making them susceptible to symmetry broken orders. Yet such surfaces have never been investigated with momentum-resolved, surface-sensitive probes, because high-temperature superconductors rarely cleave along them. Using focused-ion-beam milling to define a controlled breaking point, we expose pristine (110) side surfaces of overdoped La_2-xSr_xCuO_4 (x=0.22) suitable for angle-resolved photoemission. We observe the suppression of the superconducting spectral gap within our energy resolution (∼ 4 meV), and surprisingly, the expected zero-energy flat band peak is also suppressed, despite the high topographic quality of the surface. Self-consistent Bogoliubov–de Gennes calculations show that the measured geometric roughness of the cleaved surface is too weak to eliminate these modes. The calculations further demonstrate that bulk inhomogeneities characteristic of high-temperature superconductors, modelled as moderate Anderson-type disorder, can broaden the flat-band states beyond detectability. Our results provide the first momentum-resolved view of the electronic structure on a cuprate side surface and reveal disorder as the key factor currently preventing appearance of flat bands and their associated correlated orders.
Optimization of unconventional superconductivity involves a balance of interaction strengths. Precise determination of correlation strength across different material families is therefore important. Here, we present a combined X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS) study of infinite-layer PrNiO2 and SrCuO2 that enables fair comparison of their interaction strengths. For both compounds, we study the orbital and magnetic excitations and extract their dispersions along high-symmetry directions. Using a single-band Hubbard model and including physically plausible assumptions about higher-order exchange interactions, we estimate the correlation factor U/t for both compounds. A key finding is that despite the prediction of a smaller Coulomb repulsion U, PrNiO2 exhibits a correlation strength U/t that is 20% stronger than that of its isostructural cuprate counterpart SrCuO2. This indicates that moderation of the correlation strength may further optimize superconductivity in nickelates.
Ruddlesden-Popper (RP) nickelates have recently emerged as a new family of high-temperature superconductors. In bilayer RP nickelates, magnetic excitations with large exchange couplings have been observed, supporting a spin-mediated pairing mechanism. Whether comparable spin correlations persist in trilayer nickelates, however, remains unknown. Here, we present a Ni L-edge resonant inelastic X-ray scattering (RIXS) study of La_4Ni_3O_10 single crystals. While the orbital excitations remain similar to those of La_3Ni_2O_7, the collective spin excitations in La_4Ni_3O_10 exhibit a comparable bandwidth of about 60 meV but substantially suppressed spectral weight, implying a weaker electronic correlation in the trilayer compounds. Our results underscore the three-dimensional and multi-orbital electronic character in La_4Ni_3O_10, highlighting important differences from the bilayer nickelates. These findings provide crucial insights into the evolution of magnetism across the RP nickelate family and its connection to superconductivity.
We use uniaxial strain in combination with ultra-high-resolution resonant inelastic x-ray scattering (RIXS) at the oxygen-K and copper-L3 edges to study the excitations stemming from the charge ordering wave vector in La1.875Sr0.125CuO4. By detwinning stripe ordering, we demonstrate that the optical phonon anomalies do not show any stripe anisotropy. The low-energy charge excitations also retain an in-plane fourfold symmetry. As such, we find that both phonon and charge excitations are decoupled entirely from the strength of static charge ordering. The almost isotropic character of charge excitations is indicative of a quantum critical behavior and remains a possible source for the strange metal properties found in the normal state of cuprate superconductors.
Correlated flat bands and altermagnetism are two important directions in quantum materials, centred respectively on interaction-dominated phases and symmetry-enforced spin-textured states, yet both derive from lattice symmetry and orbital hybridization. This common origin implies that extreme crystal distortion, by narrowing bandwidths, enhancing correlations and reshaping the symmetries of altermagnetic spin splittings, could unify flat-band and altermagnetic physics in a single material; in practice, however, achieving such large distortions in a crystalline altermagnet is a formidable challenge. Here we combine a dedicated strain device with a tailored single-crystal mounting scheme to impose a highly tensile strain gradient in bulk CrSb, a prototypical altermagnet, creating a near-surface layer in which the in-plane lattice is strongly distorted relative to the weakly strained bulk, while the average bulk distortion remains small. Angle-resolved photoemission reveals a reversible regime at moderate strain, where a deeper flat-band feature, attributed to a strain-gradient-driven suppression of Cr-Sb hybridization, coexists with a correlation-enhanced Cr 3d flat band, and an irreversible regime at larger strain where partial bond decoupling drives a predominantly insulating spectral response. Density-functional calculations show that an orbital-selective altermagnetic spin texture persists across this correlated regime despite strong bandwidth renormalisation. These results define a strain-symmetry-correlation map for CrSb and establish extreme tensile strain as a route to co-engineer flat-band tendencies and spin-textured, zero-net-moment correlated states in altermagnets, pointing toward strain-adaptive, spin-selective Mott filtering and related device concepts.
The anomalous Hall effect (AHE) has emerged as a key indicator of time-reversal symmetry breaking (TRSB) and topological features in electronic band structures. Absent of a magnetic field, the AHE requires spontaneous TRSB but has proven hard to probe due to averaging over domains. The anomalous component of the Hall effect is thus frequently derived from extrapolating the magnetic field dependence of the Hall response. We show that discerning whether the AHE is an intrinsic property of the field free system becomes intricate in the presence of strong magnetic fluctuations. As a study case, we use the Weyl semimetal PrAlGe, where TRSB can be toggled via a ferromagnetic transition, providing a transparent view of the AHE's topological origin. Through a combination of thermodynamic, transport and muon spin relaxation measurements, we contrast the behaviour below the ferromagnetic transition temperature to that of strong magnetic fluctuations above. Our results on PrAlGe provide general insights into the interpretation of anomalous Hall signals in systems where TRSB is debated, such as families of Kagome metals or certain transition metal dichalcogenides.
The anomalous Hall effect (AHE) has emerged as a key indicator of time-reversal symmetry breaking (TRSB) and topological features in electronic band structures. Absent of a magnetic field, the AHE requires spontaneous TRSB but has proven hard to probe due to averaging over domains. The anomalous component of the Hall effect is thus frequently derived from extrapolating the magnetic field dependence of the Hall response. We show that discerning whether the AHE is an intrinsic property of the field-free system becomes intricate in the presence of strong magnetic fluctuations. As a study case, we use the Weyl semimetal PrAlGe, where TRSB can be toggled via a ferromagnetic transition, providing a transparent view of the AHE's topological origin. Through a combination of thermodynamic, transport, and muon spin relaxation measurements, we contrast the behavior below the ferromagnetic transition temperature to that of strong magnetic fluctuations above. Our results on PrAlGe provide general insights into the interpretation of anomalous Hall signals in systems where TRSB is debated, such as families of kagome metals or certain transition metal dichalcogenides.
The discovery of unconventional superconductivity often triggers significant interest in associated electronic and structural symmetry breaking phenomena. For the infinite-layer nickelates, structural allotropes are investigated intensively. Here, using high-energy grazing-incidence x-ray diffraction, we demonstrate how in-situ temperature annealing of the infinite-layer nickelate PrNiO2+x (x ≈ 0) induces a giant superlattice structure. The annealing effect has a maximum well above room temperature. By covering a large scattering volume, we show a rare period-six in-plane (bi-axial) symmetry and a period-four symmetry in the out-of-plane direction. This giant unit-cell superstructure—likely stemming from ordering of diffusive oxygen—persists over a large temperature range and can be quenched. As such, the stability and controlled annealing process leading to the formation of this superlattice structure provides a pathway for novel nickelate chemistry. Infinite-layer nickelates are of interest for exploration of unconventional superconductivity. Here, grazing-incidence x-ray diffraction of PrNiO2+x reveals an unusual in-plane period-six and out-of-plane period-four symmetry upon in-situ annealing, indicating a giant unit-cell superstructure.
Topological states of matter exhibit unique protection against scattering by disorder. Different topological classes exhibit distinct forms and degrees of protection. Here, we investigate the response of the ferromagnetic nodal line semimetal Fe$_3$GeTe$_2$ to disorder and electronic interactions. By combining global magneto-transport with atomic-scale scanning tunneling spectroscopy we find a simultaneous onset of diverse phenomena below a common temperature scale of about 15 K: A crossover from metallic to insulating temperature dependence of the longitudinal resistivity, saturation of the anomalous Hall conductivity to its maximal value, formation of a sharp zero-bias dip in the tunneling density of state, and emergence of multi-fractal structure of the electronic wavefunction peaking at the Fermi energy. These concurrent observations reflect the emergence of a novel energy scale possibly related to the opening of a gap in the nodal line band of Fe$_3$GeTe$_2$. Our study provides overarching insight into the role of disorder, electronic interactions and Berry curvature in setting the micro- and macro-scale responses of topological semimetals.
Multi-band Mott insulators with moderate spin-orbit and Hund's coupling are key reference points for theoretical concept developments of correlated electron systems. The ruthenate Mott insulator Ca2RuO4 has therefore been intensively studied by spectroscopic probes. However, it has been challenging to resolve the fundamental excitations emerging from the hierarchy of electronic energy scales. Here we apply high resolution resonant inelastic x-ray scattering to probe deeper into the low-energy electronic excitations found in Ca2RuO4. In this fashion, we probe a series of spin-orbital excitations. By taking advantage of enhanced energy resolution, we probe a 40 meV mode through the oxygen K-edge. The polarization dependence of this low-energy excitations exposes a distinct orbital nature, originating from the interplay of spin-orbit coupling and octahedral rotations. Additionally, we discuss the role of magnetic correlations to describe the occurrence of excitations with amplitudes which are multiple of a given energy. Such direct determination of relevant electronic energy scales sharpens the target for theory developments of Mott insulators' orbital degree of freedom.
Understanding how time-reversal symmetry (TRS) breaks in quantum materials is key to uncovering new states of matter and advancing quantum technologies. However, unraveling the interplay between TRS breaking, charge order, and superconductivity in kagome metals continues to be a compelling challenge. Here, we investigate the kagome metal Cs(V1−xNbx)3Sb5 with x = 0.07 using muon spin rotation (μSR), alternating current (AC) magnetic susceptibility, and scanning tunneling microscopy (STM), under combined tuning by chemical doping, hydrostatic pressure, magnetic field, and depth from the surface. We find that TRS breaking in the bulk emerges below 40 K—lower than the charge order onset at 58 K—while near the surface, TRS breaking onsets at 58 K and is twice as strong. Niobium doping raises the superconducting critical temperature from 2.5 K to 4.4 K. Under pressure, both the critical temperature and superfluid density double, with TRS-breaking superconductivity appearing above 0.85 GPa. These findings reveal a depth-tunable TRS-breaking state and unconventional superconducting behavior in kagome systems. Kagome systems are a rich playground to explore the interplay between superconductivity and charge order. Here, the authors present a comprehensive muon spin rotation analysis, coupled with scanning tunnelling microscopy, under various tuning parameters including chemical doping, depth and hydrostatic pressure to investigate time-reversal symmetry-breaking in Nb-doped CsV3Sb5.
Van Hove singularities (VHss) in the vicinity of the Fermi energy often play a dramatic role in the physics of strongly correlated electron materials. The divergence of the density of states generated by VHss can trigger the emergence of phases such as superconductivity, ferromagnetism, metamagnetism, and density wave orders. A detailed understanding of the electronic structure of these VHss is therefore essential for an accurate description of such instabilities. Here, we study the low-energy electronic structure of the trilayer strontium ruthenate Sr4Ru3O10, identifying a rich hierarchy of VHss using angle-resolved photoemission spectroscopy and millikelvin scanning tunneling microscopy. Comparison of k-resolved electron spectroscopy and quasiparticle interference allows us to determine the structure of the VHss and demonstrate the crucial role of spin-orbit coupling in shaping them. We use this to develop a minimal model from which we identify a mechanism for driving a field-induced Lifshitz transition in ferromagnetic metals.
Tunable quantum materials hold great potential for applications. Of special interest are materials in which small lattice strain induces giant electronic responses. The kagome compounds AV3Sb5 (A = K, Rb, Cs) provide a testbed for such singular electronic states. In this study, through angle-resolved photoemission spectroscopy, we provide comprehensive spectroscopic measurements of the giant responses induced by compressive and tensile strains on the charge-density-wave (CDW) order parameter and high-order van Hove singularity (HO-VHS) in CsV3Sb5. We observe a tripling of the CDW gap magnitudes with ~1% strain, accompanied by the changes of both energy and mass of the saddle-point fermions. Our results reveal an anticorrelation between the unconventional CDW order parameter and the mass of a HO-VHS, and highlight the role of the latter in the superconducting pairing. The giant electronic responses uncover a rich strain tunability of the versatile kagome system in studying quantum interplays under lattice perturbations.