arXiv subjects

V. Bisogni

Publications and source records attributed to V. Bisogni.

At least 19 recordsLinked to original sources

arXiv2026

Observation of multipartite spin entanglement in a cuprate chain

Quantum materials are believed to host highly entangled states of matter, but probing and quantifying such entanglement has long remained experimentally elusive. Here, we use resonant inelastic X-ray scattering (RIXS) as a probe of multipartite spin entanglement. By projecting the RIXS cross section onto the appropriate spin excitation channel, we show that the Quantum Fisher Information can be extracted directly from the measured spin fluctuation spectrum. We detect at least 7-partite spin entanglement in the model one-dimensional cuprate Sr$_2$CuO$_3$, revealing one of the largest entanglement depths yet reported in a solid. The observed entanglement depth agrees with Hubbard-model expectations and persists to elevated temperatures. Our results establish RIXS as an experimental probe of many-body spin entanglement and provide a platform for extensions to charge and orbital sectors and nonequilibrium settings.

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arXiv2026

Layer Architecture Shapes Electronic, Magnetic, and Lattice Interactions in Ruddlesden-Popper Nickelates

The discovery of superconductivity in Ruddlesden-Popper nickelates has raised a central question: how does layer architecture shape the electronic, magnetic, and lattice interactions relevant to pairing? Here, we report a detailed comparative study of the two polymorphs of La3Ni2O7--the alternating monolayer-trilayer (LNO-1313) and bilayer (LNO-2222) structures--and the related trilayer compound La4Ni3O10, using both Ni L3- and O K-edge RIXS. We find that LNO-1313 and La4Ni3O10 share strikingly similar electronic, magnetic, and lattice excitations, whereas bilayer LNO-2222 exhibits distinct features. Compared to LNO-2222, LNO-1313 and La4Ni3O10 have weaker orbital polarization, enhanced 3d8L character, a reduced out-of-plane magnetic-exchange scale, and stronger EPC. Within an effective local-moment framework, an entangled-dimer scenario provides a natural description of the spin excitations generated by strong antiferromagnetic interlayer coupling. Its advantage over conventional spin-wave theory is clearest in bilayer LNO-2222, where the interlayer coupling dominates the intralayer interactions. These findings provide critical experimental constraints for future theoretical models for the low-energy physics relevant to superconductivity in these layered nickelates.

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arXiv2026

Disentangling multi-spin dynamic correlations in the Heisenberg spin-$\frac{1}{2}$ chain

Higher-order correlations are essential for understanding exotic phases and uncovering universal aspects of quantum dynamics. While inelastic neutron scattering provides well-established access to two-particle correlations, measuring correlations in solids involving more than two particles remains a major challenge. Focusing on magnetic excitations in the Heisenberg spin-$\frac{1}{2}$ chain, we demonstrate that resonant inelastic X-ray scattering (RIXS) can selectively probe multi-spin dynamical correlations by exciting distinct intermediate states through energy detuning. Through theoretical modeling, we isolate the two- and multi- spin responses, and establish that: (i) The resonant energies of the two- and multi- spin dynamical correlations are separated by $\approx \frac{3}{4}J$; implying that the multi-spin part of the cross-section comes from intermediate states that contain spin flips; (ii) The spectral weight of the two-spin channel exhibits a Lorentzian resonant energy profile consistent with a single dominant electronic configuration, whereas the multi-spin channel response shows a Gaussian-like profile, implying contributions from multiple intermediate spin configurations. These characteristics are reproduced by exact diagonalization of the $t-J$ Hamiltonian, which further reveals that the widths of Lorentzian and Gaussian resonant energy profiles depend primarily on core-hole lifetime ($\Gamma/2$) and $\frac{2J}{\Gamma}$, respectively. Controlled access to multi-spin dynamics, using RIXS energy detuning as a knob, can open new pathways to explore many-body dynamics in quantum materials.

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arXiv2026

Observation of correlated plasmons in low-valence nickelates

The discovery of nickelate superconductors has opened a new arena for studying the behavior of correlated electron liquids that give rise to unconventional superconductivity. While critical information about a material's charge dynamics is encoded in its plasmons, collective modes of the electron gas, these excitations have not yet been observed in nickelate materials. Here, we use resonant inelastic x-ray scattering (RIXS) to detect plasmons in the metallic, low-valence nickelate Pr4Ni3O8. Although qualitatively similar to those in cuprates, the nickelate plasmons are more heavily damped and have a lower velocity than those in a cuprate at comparable doping, which we attribute to reduced electronic hopping and enhanced screening of the long-range Coulomb interactions. Furthermore, the plasmons in Pr4Ni3O8 soften with increasing temperature, in contrast to the cuprate, where plasmons remain at nearly fixed energy but become more strongly damped. Taken together, these results reveal a distinct charge-screening landscape in nickelates and place quantitative constraints on analogies to cuprates.

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arXiv2026

Stability of the Local Ni$^{2+}$ Electronic Structure to $A$-site Disorder in the Pyrochlore Antiferromagnet NaCaNi$_2$F$_7$

NaCaNi$_2$F$_7$ is a unique example of spin-1 Heisenberg antiferromagnet on the pyrochlore lattice, but the presence of Na$^{1+}$/Ca$^{2+}$ $A$-site disorder complicates the local electronic and magnetic environment of the Ni$^{2+}$ $B$-site. We utilize resonant inelastic X-ray scattering (RIXS) to study the influence of $A$-site disorder on the $B$-site electronic structure of NaCaNi$_2$F$_7$. Ni L-edge RIXS measurements reveal a Ni$^{2+}$ electronic structure in nearly ideal octahedral coordination, with only a small trigonal compression ($δ$ = -200$\;$meV) required to capture all spectral features. Within the $D_{3d}$ symmetry of the Ni local environment, we extract an anisotropic $g$-factor of $g_{\parallel} = 2.26$ and $g_{\perp} = 2.27$, and a corresponding paramagnetic moment of $μ_{\rm{eff}}=3.2\;μ_B$. To simulate disorder, RIXS spectra were calculated with realistic distributions of crystal field parameters; however, these spectra are invariant relative to a disorder-free model, demonstrating the robustness of the Ni$^{2+}$ electronic environment to the $A$-site disorder, within the resolution of our measurement.

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arXiv2025

Observation of anisotropic dispersive dark exciton dynamics in CrSBr

Many-body excitons in CrSBr are attracting intense interest in view of their highly anisotropic magneto-optical coupling and their potential for novel optical interfaces within spintronic and magnonic devices. Characterizing the orbital character and propagation of these electronic excitations is crucial for understanding and controlling their behavior; however, this information is challenging to access. Ultra-high resolution resonant inelastic x-ray scattering is a momentum-resolved technique that can address these crucial questions. We present measurements collected at the Cr $L_3$-edge which show a rich spectrum of excitations with a variety of spin-orbital characters. While most of these excitations appear to be localized, the dispersion of the lowest energy dark exciton indicates that it is able to propagate along both the $a$ and $b$ directions within the planes of the crystal. This two-dimensional character is surprising as it contrasts with electrical conductivity and the behavior of the bright exciton, both of which are strongly one-dimensional. The discovery of this propagating dark exciton highlights an unusual coexistence of one- and two-dimensional electronic behaviors in CrSBr.

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arXiv2025

Magnetic excitations and absence of charge order in the van der Waals ferromagnet Fe$_{4.75}$GeTe$_2$

Understanding the ground state of van der Waals (vdW) magnets is crucial for designing devices leveraging these platforms. Here, we investigate the magnetic excitations and charge order in Fe$_{4.75}$GeTe$_2$, a vdW ferromagnet with $\approx$ 315 K Curie temperature. Using Fe $L_3 - $edge resonant inelastic x-ray scattering, we observe a dual nature of magnetic excitations, comprising a coherent magnon and a broad non-dispersive continuum extending up to 150 meV, 50$\%$ higher than in Fe$_{2.72}$GeTe$_2$. The continuum intensity is sinusoidally modulated along the stacking direction $L$, with a period matching the inter-slab distance. Our results indicate that while the dual character of the magnetic excitations is generic to Fe-Ge-Te vdW magnets, Fe$_{4.75}$GeTe$_2$ exhibits a longer out-of-plane magnetic correlation length, suggesting enhanced 3D magnetic character. Furthermore, resonant x-ray diffraction reveals that previously reported $\pm$(1/3, 1/3, $L$) peaks originate from crystal structure rather than from charge order.

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arXiv2025

Evidence of electronic states driving current-induced insulator-to-metal transition

On demand current-driven insulator-to-metal transition (IMT) is pivotal for the next generation of energy-efficient and scalable microelectronics. IMT is a key phenomenon observed in various quantum materials, and it is enabled by the complex interplay of spin, lattice, charge, and orbital degrees of freedom (DOF). Despite significant prior work, the underlying mechanism of the current-driven IMT remains elusive, primarily due to the difficulty in simultaneously obtaining bulk fingerprints of all the electronic DOF. Here, we employ in-operando resonant inelastic x-ray scattering (RIXS) on Ca$_2$RuO$_4$, a prototypical strongly correlated material, to track the evolution of the electronic DOF encoded in the RIXS spectra during the current-driven IMT. Upon entering the conductive state, we observe an energy-selective suppression of the RIXS intensity, proportional to the current. Using complementary RIXS cross-section calculations, we demonstrate that the non-equilibrium conductive state emerges from the formation of correlated electronic states with a persistent Mott gap.

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arXiv2025

Dispersive dark excitons in van der Waals ferromagnet CrI3

Spin-flip dark excitons are optical-dipole-forbidden quasiparticles with remarkable potential in optoelectronics, especially when they are realized within cleavable van der Waals materials. Despite this potential, dark excitons have not yet been definitively identified in ferromagnetic van der Waals materials. Here, we report two dark excitons in a model ferromagnetic material CrI3 using high-resolution resonant inelastic x-ray scattering (RIXS) and show that they feature narrower linewidths compared to the bright excitons previously reported in this material. These excitons are shown to have spin-flip character, to disperse as a function of momentum, and to change through the ferromagnetic transition temperature. Given the versatility of van der Waals materials, these excitons hold promise for new types of magneto-optical functionality.

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arXiv2024

Superconductivity in the parent infinite-layer nickelate NdNiO$_2$

We report evidence for superconductivity with onset temperatures up to 11 K in thin films of the infinite-layer nickelate parent compound NdNiO$_2$. A combination of oxide molecular-beam epitaxy and atomic hydrogen reduction yields samples with high crystallinity and low residual resistivities, a substantial fraction of which exhibit superconducting transitions. We survey a large series of samples with a variety of techniques, including electrical transport, scanning transmission electron microscopy, x-ray absorption spectroscopy, and resonant inelastic x-ray scattering, to investigate the possible origins of superconductivity. We propose that superconductivity could be intrinsic to the undoped infinite-layer nickelates but suppressed by disorder due to its nodal order parameter, a finding which would necessitate a reconsideration of the nickelate phase diagram. Another possible hypothesis is that the parent materials can be hole doped from randomly dispersed apical oxygen atoms, which would suggest an alternative pathway for achieving superconductivity.

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arXiv2024

Capping effects on spin and charge excitations in parent and superconducting Nd1-xSrxNiO2

Superconductivity in infinite layer nickelates Nd1-xSrxNiO2 has so far been achieved only in thin films raising questions on the role of substrates and interfaces. Given the challenges associated with their synthesis it is imperative to identify their intrinsic properties. We use Resonant Inelastic X-ray Scattering (RIXS) to investigate the influence of the SrTiO3 capping layer on the excitations of Nd1-xSrxNiO2 (x = 0 and 0.2). Spin excitations are observed in parent and 20% doped Nd1-xSrxNiO2 regardless of capping, proving that magnetism is intrinsic to infinite-layer nickelates and appears in a significant fraction of their phase diagram. In parent and superconducting Nd1-xSrxNiO2, the spin excitations are slightly hardened in capped samples compared to the non-capped ones. Additionally, a weaker Ni - Nd charge transfer peak at ~ 0.6 eV suggests that the hybridization between Ni 3d and Nd 5d orbitals is reduced in capped samples. From our data, capping induces only minimal differences in Nd1-xSrxNiO2 and we phenomenologically discuss these differences based on the reconstruction of the SrTiO3 - NdNiO2 interface and other mechanisms such as crystalline disorder.

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arXiv2024

Magnetically propagating Hund's exciton in van der Waals antiferromagnet NiPS3

Magnetic van der Waals (vdW) materials have opened new frontiers for realizing novel many-body phenomena. Recently NiPS3 has received intense interest since it hosts an excitonic quasiparticle whose properties appear to be intimately linked to the magnetic state of the lattice. Despite extensive studies, the electronic character, mobility, and magnetic interactions of the exciton remain unresolved. Here we address these issues by measuring NiPS3 with ultra-high energy resolution resonant inelastic x-ray scattering (RIXS). We find that Hund's exchange interactions are primarily responsible for the energy of formation of the exciton. Measuring the dispersion of the Hund's exciton reveals that it propagates in a way that is analogous to a double-magnon. We trace this unique behavior to fundamental similarities between the NiPS3 exciton hopping and spin exchange processes, underlining the unique magnetic characteristics of this novel quasiparticle.

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arXiv2023

Comment on newly found Charge Density Waves in infinite layer Nickelates

Recent works[1-3] reported evidence for charge density waves (CDWs) in infinite layer nickelates (112 structure) based on resonant diffraction at the Ni $L_3$ edge measured at fixed scattering angle. We have found that a measurement with fixed momentum transfer, rather than scattering angle, does not show a resonance effect. We have also observed that a nearby structural Bragg peak from the substrate appears due to third harmonic content of the incident beam, and spreads intensity down to the region of the attributed CDW order. This was further confirmed by testing a bare substrate. We suggest procedures to confirm an effective resonant enhancement of a diffraction peak.

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arXiv2023

Resonant inelastic x-ray scattering data for Ruddlesden-Popper and reduced Ruddlesden-Popper nickelates

Ruddlesden-Popper and reduced Ruddlesden-Popper nickelates are intriguing candidates for mimicking the properties of high-temperature superconducting cuprates. The degree of similarity between these nickelates and cuprates has been the subject of considerable debate. Resonant inelastic x-ray scattering (RIXS) has played an important role in exploring their electronic and magnetic excitations, but these efforts have been stymied by inconsistencies between different samples and the lack of publicly available data for detailed comparison. To address this issue, we present open RIXS data on La4Ni3O10 and La4Ni3O8.

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arXiv2023

Low-energy quasi-circular electron correlations with charge order wavelength in $\textrm{Bi}_2\textrm{Sr}_2\textrm{Ca}\textrm{Cu}_2\textrm{O}_{8+δ}$

In the study of dynamic charge order correlations in the cuprates, most high energy-resolution resonant inelastic x-ray scattering (RIXS) measurements have focused on momenta along the high-symmetry directions of the copper oxide plane. However, electron scattering along other in-plane directions should not be neglected as they may contain information relevant, for example, to the origin of charge order correlations or to our understanding of the isotropic scattering responsible for strange metal behavior in cuprates. We report high-resolution resonant inelastic x-ray scattering (RIXS) experiments that reveal the presence of dynamic electron correlations over the $q_x$-$q_y$ scattering plane in underdoped $\textrm{Bi}_2\textrm{Sr}_2\textrm{Ca}\textrm{Cu}_2\textrm{O}_{8+δ}$ with $T_c=54$ K. We use the softening of the RIXS-measured bond stretching phonon line as a marker for the presence of charge-order-related dynamic electron correlations. The experiments show that these dynamic correlations exist at energies below approximately $70$ meV and are centered around a quasi-circular manifold in the $q_x$-$q_y$ scattering plane with radius equal to the magnitude of the charge order wave vector, $q_{CO}$. We also demonstrate how this phonon-tracking procedure provides the necessary experimental precision to rule out fluctuations of short-range directional charge order (i.e. centered around $[q_x=\pm q_{CO}, q_y=0]$ and $[q_x=0, q_y=\pm q_{CO}]$) as the origin of the observed correlations.

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arXiv2023

Electronic character of charge order in square planar low valence nickelates

Charge order is a central feature of the physics of cuprate superconductors and is known to arise from a modulation of holes with primarily oxygen character. Low-valence nickelate superconductors also host charge order, but the electronic character of this symmetry breaking is unsettled. Here, using resonant inelastic x-ray scattering at the Ni $L_2$-edge, we identify intertwined involvements of Ni $3d_{x^2-y^2}$, $3d_{3z^2-r^2}$, and O $2p_σ$ orbitals in the formation of diagonal charge order in an overdoped low-valence nickelate La$_{4}$Ni$_{3}$O$_{8}$. The Ni $3d_{x^2-y^2}$ orbitals, strongly hybridized with planar O $2p_σ$, largely shape the spatial charge distribution and lead to Ni site-centered charge order. The $3d_{3z^2-r^2}$ orbitals play a small, but non-negligible role in the charge order as they hybridize with the rare-earth $5d$ orbitals. Our results reveal that the low-energy physics and ground-state character of these nickelates are more complex than those in cuprates.

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arXiv2022

Electronic structure of the frustrated diamond lattice magnet NiRh$_2$O$_4$

The $A$-site spinel NiRh$_2$O$_4$ is the only known realization of a spin-1 diamond lattice magnet and is predicted to host unconventional magnetic phenomena driven by frustrated nearest and next-nearest neighbor exchange as well as orbital degeneracy. Previous works found no sign of magnetic order but found a gapped dispersive magnetic excitation indicating a possible valence bond magnetic ground state. However, the presence of many competing low energy degrees of freedom and limited empirical microscopic constraints complicates further analysis. Here, we carry out resonant inelastic x-ray scattering (RIXS) and x-ray absorption spectroscopy (XAS) to characterize the local electronic structure of NiRh$_2$O$_4$. The RIXS data can be partly described by a single-ion model for tetrahedrally coordinated Ni$^{2+}$ and indicates a tetragonal distortion $Δt_2\!=\!70$ meV that splits the $t_2$ orbitals into a high energy orbital singlet and lower energy orbital doublet. We identify features of the RIXS spectra that are consistent with a Rh-Ni two-site excitation indicating strong metal-metal hybridization mediated by oxygen in NiRh$_2$O$_4$. We also identify signatures of electron-phonon coupling through the appearance of phonon sidebands that dress crystal field excitations. These results establish the key energy scales relevant to the magnetism in NiRh$_2$O$_4$ and further demonstrate that covalency and lattice dynamics play essential roles in controlling the magnetic ground states of $A$-site spinels.

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arXiv2022

Role of Oxygen States in the Low Valence Nickelate La$_4$Ni$_3$O$_8$

The discovery of superconductivity in square-planar low valence nickelates has ignited a vigorous debate regarding their essential electronic properties: Do these materials have appreciable oxygen charge-transfer character akin to the cuprates, or are they in a distinct Mott-Hubbard regime where oxygen plays a minimal role? Here, we resolve this question using O $K$-edge resonant inelastic x-ray scattering (RIXS) measurements of the low valence nickelate La$_{4}$Ni$_{3}$O$_{8}$ and a prototypical cuprate La$_{2-x}$Sr$_{x}$CuO$_{4}$ ($x=0.35$). As expected, the cuprate lies deep in the charge-transfer regime of the Zaanen-Sawatzky-Allen scheme. The nickelate, however, is not well described by either limit of the ZSA scheme and is found to be of mixed charge-transfer/Mott-Hubbard character with the Coulomb repulsion $U$ of similar size to the charge-transfer energy $Δ$. Nevertheless, the transition-metal-oxygen hopping is larger in La$_{4}$Ni$_{3}$O$_{8}$ than in La$_{2-x}$Sr$_{x}$CuO$_{4}$, leading to a significant superexchange interaction and an appreciable hole occupation of the ligand O orbitals in La$_{4}$Ni$_{3}$O$_{8}$ despite its larger $Δ$. Our results clarify the essential characteristics of low valence nickelates and put strong constraints on theoretical interpretations of superconductivity in these materials.

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