We compute high-resolution angle-resolved photoemission spectroscopy of the Hubbard model using the unbiased determinant quantum Monte Carlo algorithm, revealing an asymmetry between electron and hole doping. Electron doping exhibits more coherent quasiparticles and stronger antiferromagnetic correlations compared to hole doping. At low doping, a nodal-antinodal dichotomy on the Fermi surface is observed, similar to cuprate experiments. The dichotomy reflects the momentum dependence of the Mott gap, as manifested in both the spectral function and the self-energy. For hole doping, we observe a transition towards the pseudogap, without signature of pocket formation. The simulated nuclear magnetic resonance pseudogap temperatures do not necessarily agree with the temperature determined by spectroscopy. These findings collectively suggest the pseudogap is a smooth crossover driven by strong correlations.

The quality of numerically simulated spectra using real-time evolution methods for strongly correlated systems is affected by both the length of simulation time and the system size, limiting resolution in both frequency and momentum. In this work, we propose a computationally cheap, linear autoregressive machine learning-based framework to extend short-time and short-distance results over a wider range. We use the proposed method to extend the lesser Green’s function for both the Hubbard model and the much more computationally challenging Hubbard-extended Holstein model. This technique significantly improves both the frequency and momentum resolution of the single-particle removal spectrum $${\mathcal{A}}(k,\omega )$$, allowing the observation of otherwise obscured spectral features due to electron-phonon coupling.

We demonstrate control of helimagnetic order in biaxially strained SrFeO3 thin films using neutron diffraction and resonant soft x-ray scattering. SrFeO3, a negative charge-transfer oxide, exhibits a complex magnetic phase diagram that includes multi-q spin structures. Tensile epitaxial strain produces a pronounced shortening of the helimagnetic ordering length and a tilting of the magnetic ordering vector. We interpret this behavior in terms of chemical expansion: lattice dilation under tensile strain lowers the energetic cost of oxygen vacancies, leading to an expanded unit cell that modifies Fe-O hybridization and enhances superexchange relative to double exchange. These results reveal how epitaxial strain can indirectly tune helimagnetism through defect-driven chemical expansion, highlighting the strong coupling between lattice, chemistry, and magnetic order in transition-metal oxides. Our findings establish chemical expansion as an effective mechanism for engineering complex magnetic textures in oxide thin films, with implications for spintronic, magnonic, and quantum information applications.

The single-band Hubbard model is one of the most extensively studied models in condensed matter physics, giving rise to intertwined spin and charge stripes that coexist with, or lie in the vicinity of, superconductivity in the phase diagram. However, whether the low energy physics of the single-band Hubbard model is fully equivalent to the multi-band (multi-orbital) Emery model remains an unsettled question. While the intertwined stripes and nematicity have been studied in the single-band Hubbard model, a comprehensive picture in the Emery model is lacking. In this paper, we focus on the less investigated intertwined charge stripes using complementary density matrix renormalization group (DMRG) and determinant quantum Monte Carlo (DQMC) techniques. Our ground state DMRG confirms the presence of the oxygen-centered charge stripes at a reduced amplitude in the Emery model parameter regime widely used in the study of intertwined stripes. Close analysis of the oxygen orbital structure of the static charge correlation function from DQMC reveals the charge stripe pattern in real-space, showcasing stronger charge density modulation on p-orbitals pointing along “the rivers of charge”, consistent with DMRG. For the parameter set with the largest fermion signs, we managed to reach a temperature where the system first demonstrated tendencies to form purely unidirectional spin and charge stripes, and the B_1g component becomes dominant in the bond-charge nematic susceptibility. This observation correlates with the doping dependence of the kinetic energy anisotropy, suggesting a close relation between the nematicity and charge stripes in the Emery model.

The discovery of high-T_c superconductivity in Ruddlesden-Popper nickelates has sparked substantial effort towards understanding unconventional electronic states beyond a traditional cuprate-like d^9 configurational ground state. An understanding of the interplay between magnetic ground states and multi-orbital physics is key for establishing a microscopic mechanism for superconductivity. In the bilayer nickelates, spin density wave (SDW) order is a prominent feature in the non-superconducting regime, yet its relation to superconducting pairing remains an open question. Here, we use resonant x-ray scattering to examine the existence of SDW order in superconducting bilayer nickelate thin films La_2PrNi_2O_7 (LPNO). Comparing superconducting and oxygen-deficient LPNO thin films, we find that superconductivity occurs in SDW-free, oxygen-stoichiometric regions, whereas oxygen-deficiency promotes SDW order, indicating phase segregation of SDW and superconductivity. Furthermore, Ni-L_3 and O-K edge spectroscopy reveals distinct electronic structures - particularly along the c-axis - between the two regions. Our results identify oxygen stoichiometry as a key parameter controlling interlayer coupling and thus the electronic structure of bilayer nickelates. In concert with theory, we propose that a ligand hole primarily resides at the inter-bilayer apical oxygen, forming a robust interlayer five-spin polaron state, which serves as the ground state for superconducting bilayer nickelates.

Elucidating the microscopic behavior of cuprates under ultrafast photoexcitation offers critical insights into their highly correlated out-of-equilibrium states. Although quasiparticle dynamics have been investigated extensively, the behavior of collective magnetic excitations remains comparatively unexplored. Here, we use time-resolved resonant inelastic X-ray scattering (trRIXS) at the Cu L_3-edge to track the collective magnetic excitations (paramagnons) in an optimally electron-doped cuprate driven out-of-equilibrium by a femtosecond pump laser pulse. Upon pumping, we observed an anti-Stokes signal associated with paramagnon generation, which modifies the paramagnon dispersion near the zone center, although the bandwidth remained unchanged. Moreover, the spectral weight exhibits a momentum-dependent variation across the Brillouin zone. The light-driven boost of the paramagnon population and the resulting spectral-weight transfer could provide new leverage to manipulate the properties of cuprates.

Understanding the excitations of quantum materials is essential for unraveling how their microscopic constituents interact. Among these, particle-hole excitations form a particularly important class, as they govern fundamental processes such as screening, dissipation, and transport. In metals, the continuum of electron-hole excitations is described by the Lindhard function. Although central to the theory of Fermi liquids, the corresponding Lindhard continuum has remained experimentally elusive. Here, we report its direct observation in the weakly correlated metal MgB_2 using ultra-soft resonant inelastic X-ray scattering (RIXS). We resolve a linearly dispersing excitation with velocity comparable to the Fermi velocity and find quantitative agreement with simulations of the non-interacting charge susceptibility. A detailed analysis and decomposition of the simulations reveal the intra-band origin of this low-energy excitation, confirming it as the Lindhard continuum. Our results establish ultra-soft RIXS as a momentum-resolved probe of the fermiology in metals and call for deeper investigations of continuum features in RIXS and related spectroscopy of other materials beyond MgB_2.

X-ray spectroscopy has been a key method to determine ground and excited state properties of quantum materials with atomic specificity. Now, new x-ray facilities are opening the door to the study of pump-probe x-ray spectroscopy - specifically time-resolved x-ray absorption (trXAS) and time-resolved resonant inelastic x-ray scattering (trRIXS). In this paper we will present simulations of each of these spectroscopies using a time-domain full atomic multiplet, charge transfer Hamiltonian, adapted to study the properties of a generalized cluster model including a central transition metal ion caged by ligand atoms in a planar geometry. The numerically evaluated trXAS and trRIXS cross-sections for representative electron configurations 3d^9 and 3d^8 demonstrate the insights that can be obtained from charge transfer pumping, and how this nonequilibrium process affects ground and excited state properties. The straightforward characterization of the excitations in these systems, based on our analysis of the simulations, can serve as a benchmark for future experiments, as access to these time-resolved spectroscopic techniques becomes more widely available.

We present results of a Raman scattering study of the Kagome ferromagnet Co_3Sn_2S_2, with a focus on electronic and phononic excitations and their interplay. We provide a theoretical analysis of the electronic band structure, enabling a semi-quantitative explanation of the spectra. A prominent feature in the electronic spectra is a redistribution of spectral weight from low to high energies in all polarization configurations starting at the Curie temperature T_C. In the symmetry-resolved spectra, the suppression of the A_1g continuum in the ferromagnetic state arises from the redistribution of electronic states below T_C, while a strong enhancement of the A_2g continuum is linked to the dynamics of fermions near the Fermi level E_ F being characterized by spin-momentum locking near Weyl points. The A_1g phonon modulates the position of these Weyl points and couples strongly to the related fermions close to E_ F. These results allow a comprehensive understanding of the bulk band structure evolution as a function of temperature in Co_3Sn_2S_2, offering key insights for further studies of the driving force behind the long-range magnetic order and novel topological states in this compound.

The layered cobaltate CaCoO2 exhibits a unique herringbone-like structure. Serving as a potential prototype for a new class of complex lattice patterns, we study the properties of CaCoO2 using X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS). Our results reveal a significant inter-plane hybridization between the Ca 4s- and Co 3d- orbitals, leading to an inversion of the textbook orbital occupation of a square planar geometry. Further, our RIXS data reveal a strong low energy mode, with anomalous intensity modulations as a function of momentum transfer close to a quasi-static response. These findings indicate that the newly discovered herringbone structure exhibited in CaCoO2 may serve as a promising laboratory for the design of materials having strong electronic, orbital and lattice correlations.

Numerical evidence for superconductivity in the single-band Hubbard model is elusive or ambiguous despite extensive study, raising the question of whether the single-band Hubbard model is a faithful low energy effective model for cuprates, and whether explicitly including the oxygen ions will recover the properties necessary for superconducting transition. Here we show, by using numerically exact determinant quantum Monte Carlo (DQMC) simulations of the doped two-dimensional three-band Emery model, that while the single-band model exhibits strikingly T-linear transport behavior, the three-band model shows a low temperature resistivity curvature indicating a crossover to a more metallic transport regime. Evidence has also been found in thermodynamic and superconducting measurements, which suggests that some degree of coherence in transport might be necessary for the high-temperature superconductivity in cuprates, further implying a possible connection between superconducting and transport behaviors.

Recent studies of La_{3}Ni_{2}O_{7} have identified a bilayer (2222) structure and an unexpected alternating monolayer-trilayer (1313) structure, both of which feature signatures of superconductivity near 80 K under high pressures. Using angle-resolved photoemission spectroscopy, we measure the electronic structure of 1313 samples. In contrast to the previously studied 2222 structure, we find that the 1313 structure hosts a flat band with a markedly different binding energy, as well as an additional electron pocket and band splittings. By comparison to local-density approximation calculations, we find renormalizations of the Ni-d_{z^{2}} and Ni-d_{x^{2}-y^{2}} derived bands to be about 5 to 7 and about 4, respectively, suggesting strong correlation effects. These results reveal important differences in the electronic structure brought about by the distinct structural motifs with the same stoichiometry. Such differences may be relevant to the putative high temperature superconductivity.

Iron redox cycling between low-valent oxidation states of FeII and FeIII drives crucial processes in nature. The FeII/III redox couple charge compensates the cycling of lithium iron phosphate, a positive electrode (cathode) for lithium-ion batteries. High-valent iron redox couples, involving formal oxidation higher than FeIII, could deliver higher electrochemical potentials and energy densities. However, because of the instability of high-valent Fe electrodes, they have proven difficult to probe and exploit in intercalation systems. Here we report and characterize a formal FeIII/V redox couple by revisiting the charge compensation mechanism of (de)lithiation in Li4FeSbO6. Valence-sensitive experimental and computational core-level spectroscopy reveal a direct transition from FeIII (3d5) to a negative-charge-transfer FeV (3d5L2) ground state on delithiation, without forming FeIV, or oxygen dimers. We identify that the cation ordering in Li4FeSbO6 drives a templated phase transition to stabilize the unique FeV species and demonstrate that disrupting cation ordering suppresses the FeIII/V redox couple. Exhibiting resistance to calendar aging, high operating potential and low voltage hysteresis, the FeIII/V redox couple in Li4FeSbO6 provides a framework for developing sustainable, Fe-based intercalation cathodes for high-voltage applications.

Modern energy applications, especially electric vehicles, demand high energy batteries. However, despite decades of intensive efforts, the highest energy density and commercially viable batteries are still based on LiCoO2, the very first generation of cathode materials. The technical bottleneck is the stability of oxide-based cathodes at high operating voltages. The fundamental puzzle is that we actually never understood the redox mechanism of LiCoO2. Conventional wisdom generally defines redox to be centered on cations at low voltages, and on anions, i.e. oxygen, at high voltages by forming oxidized chemical states like O2 or peroxo-species. Here, through in-situ and ex-situ spectroscopy coupled with theoretical calculations, we show that high-energy layered cathodes, represented by LiCoO2 and LiNiO2, operate through enhancement of negative charge transfer (NCT) ground states upon charging throughout the whole voltage range - i.e., NCT evolution itself is the intrinsic redox mechanism regardless of voltage ranges. NCT inherently engages high covalency and oxygen holes, leading to optimized performance without conventional redox centers in LiCoO2. The level of NCT, i.e., number of ligand holes, naturally explains many seemingly controversial results. The redefinition of redox mechanism reveals the pathway toward viable high energy battery electrodes.

In light of recent experimental data indicating a substantial thermal Hall effect in square lattice antiferromagnetic Mott insulators, we investigate whether a simple Mott insulator can sustain a finite thermal Hall effect. We verify that the answer is "no" if one performs calculations within a spin-only lowenergy effective spin model with noninteracting magnons. However, by performing determinant quantum Monte Carlo simulations, we show the single-band t-t'-U Hubbard model coupled to an orbital magnetic field does support a finite thermal Hall effect when t' # 0 and B # 0 in the Mott insulating phase. We argue that the (carrier agnostic) necessary conditions for observing a finite thermal Hall effect are time-reversal and particle-hole symmetry breaking. By considering magnon-magnon scattering using a semiclassical Boltzmann analysis, we illustrate a physical mechanism by which finite transverse thermal conductivity may arise, consistent with our symmetry argument and numerical results. Our results indicate that square and triangular lattices with SU(2) symmetry can support a finite thermal Hall effect and call for a critical reexamination of thermal Hall effect data in insulating magnets, as the magnon contribution should not be excluded a priori.

Topologically ordered states, such as chiral spin liquids, have been proposed as candidates that host fractionalized excitations. However, detecting chiral character or proximity to these non-trivial states remains a challenge. Resonant Raman scattering can be a powerful tool for detecting chiral fluctuations, as the A_2g channel probes excitations with broken time-reversal symmetry and local chiral order. Here, we use exact diagonalization to characterize the resonant A_2g channel, alongside two-magnon scattering in B_1g and E_g channels, for the Hubbard model on lattices with increasing levels of geometric spin frustration, where tuning the incident energy near the Mott gap reveals strong chiral spin excitation intensity. Increased spin frustration in the Mott insulator results in an overall softening of the Raman A_2g response, indicating a tendency toward low energy chiral-chiral fluctuations in Mott insulators with magnetic frustration and proximity to chiral spin liquid states that can potentially be tuned by external perturbations.

Recent photoemission experiments on the quasi-one-dimensional Ba-based cuprates suggest that doped holes experience an attractive potential not captured using the simple Hubbard model. This observation has garnered significant attention due to its potential relevance to Cooper pair formation in high-T_c cuprate superconductors. To scrutinize this assertion, we examined signatures of such an attractive potential in doped 1D cuprates Ba_2CuO_3+δ by measuring the dispersion of the 2-spinon excitations using Cu L_3-edge resonant inelastic X-ray scattering (RIXS). Upon doping, the 2-spinon excitations appear to weaken, with a shift of the minimal position corresponding to the nesting vector of the Fermi points, q_F. Notably, we find that the energy scale of the 2-spinons near the Brillouin zone boundary is substantially softened compared to that predicted by the Hubbard model in one-dimension. Such a discrepancy implies missing ingredients, which lends support for the presence of an additional attractive potential between holes.

We performed angle-resolved photoemission spectroscopy studies on the triple-layer Bi2Sr2Ca2Cu3O10+δ over a wide doping range. Although the doping level of the inner CuO2 plane is extremely low in underdoped samples, the d-wave SC gap is enhanced to the unprecedentedly large value of Δ0 ~ 80-100 meV at the antinode. This gap persists well above Tc without a Fermi arc, indicating a "nodal metal". We attribute the nodal metallic behavior to the unique local environment of the inner clean CuO2 plane, sandwiched by nearly optimally-doped two outer planes and hence subject to strong proximity effect from both sides. In the nodal metal, quasiparticle peaks show electron-hole symmetry, suggesting d-wave pairing fluctuations. Thus the proximity effect on the innermost CuO2 plane is the strongest in the triple-layer cuprates, which explains why the Tc reaches the maximum at the layer number of three in every multi-layer cuprate family.

Quasi-one-dimensional (1D) materials provide a unique platform for understanding the importance and influence of extended interactions on the physics of strongly correlated systems due to their relative structural simplicity and the existence of powerful theoretical tools well adapted to one spatial dimension. Recently, this was highlighted by anomalous observations in the single-particle spectral function A(q, w) of 1D cuprate chain compounds, measured by angle-resolved photoemission spectroscopy (ARPES), which were explained by the presence of a long-range attractive interaction. Such an extended interaction should leave its fingerprints on other observables, notably the dynamical spin structure factor S(q, w), measured by neutron scattering or resonant inelastic x-ray scattering. Starting from a simple Hubbard Hamiltonian in 1D and using time-dependent density matrix renormalization group methods, we show that the presence of long-range attractive coupling, directly through an instantaneous Coulomb interaction V or retarded electron-phonon (el-ph) coupling, can introduce significant spectral weight redistribution in S(q, w) across a wide range of doping. This underscores the significant impact that extended interactions can have on dynamical correlations among particles, and the importance of properly incorporating this influence in modeling. Our results demonstrate that S(q, w) can provide a sensitive experimental constraint, which complements ARPES measurements, in identifying key interactions in 1D cuprates, beyond the standard Hubbard model.