arXiv subjects

M. Mitrano

Publications and source records attributed to M. Mitrano.

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.

cond-mat.str-el↗

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.

cond-mat.str-el↗

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.

cond-mat.str-el↗

arXiv2026

Quantum control of Hubbard excitons

Quantum control of the many-body wavefunction is a central challenge in quantum materials research, as it could yield a precise control knob to manipulate emergent phenomena. Floquet engineering, the coherent dressing of quantum states with periodic non-resonant optical fields, has become an important strategy for quantum control. Most applications to solid-state systems have targeted weakly interacting or single-ion states, leaving the manipulation of many-body wavefunctions largely unexplored. Here, we use Floquet engineering to achieve quantum control of a strongly correlated Hubbard exciton in the one-dimensional Mott insulator Sr$_2$CuO$_3$. A nonresonant midinfrared optical field coherently dresses the exciton wavefunction, driving its rotation between bright and dark states. We use resonant third-harmonic generation to quantify ultrafast $\pi/2$ rotations on the Bloch sphere spanned by these exciton states. Our work advances the quest towards programmable control of correlated states and exciton-based quantum sensing.

cond-mat.str-el↗

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.

cond-mat.str-el↗

arXiv2025

Photoinduced Frustration Modulation in $\kappa$-type Quantum Spin Liquid Candidates

Geometric frustration is a key parameter controlling electronic and magnetic properties of quantum spin liquid systems, yet remains challenging to tune. Here, we coherently drive molecular vibrations with midinfrared pulses in two organic quantum spin liquid candidates, the insulating $\kappa$-(BEDT-TTF)$_2$Cu$_2$(CN)$_3$ and the metallic $\kappa$-(BEDT-TTF)$_4$Hg$_{2.89}$Br$_8$, and probe their electronic response through ultrafast reflectivity measurements. We observe a nonlinear coupling between local molecular vibrations and nonlocal phonons, which is expected to directly modulate the geometric frustration of their triangular lattice. Our findings establish a promising route to dynamically control frustration in nonbipartite quantum materials.

cond-mat.str-el↗

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.

cond-mat.str-el↗

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.

cond-mat.str-el↗

arXiv2024

Exploring Quantum Materials with Resonant Inelastic X-Ray Scattering

Understanding quantum materials -- solids in which quantum-mechanical interactions among constituent electrons yield a great variety of novel emergent phenomena -- is a forefront challenge in modern condensed matter physics. This goal has driven the invention and refinement of several experimental methods, which can spectroscopically determine the elementary excitations and correlation functions that determine material properties. This Perspectives article focuses on the future experimental and theoretical trends of resonant inelastic x-ray scattering (RIXS), which is a remarkably versatile and rapidly growing technique for probing different charge, lattice, spin, and orbital excitations in quantum materials. We provide a forward-looking introduction to RIXS and outline how this technique is poised to deepen our insight into the nature of quantum materials and their emergent electronic phenomena.

cond-mat.str-el↗

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.

cond-mat.str-el↗

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 $2p_{\sigma}$ 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 $2p_{\sigma}$, 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.

cond-mat.str-el↗

arXiv2021

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 $\Delta$. 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 $\Delta$. Our results clarify the essential characteristics of low valence nickelates and put strong constraints on theoretical interpretations of superconductivity in these materials.

cond-mat.supr-con↗

arXiv2020

Observation of Pines' Demon in Sr$_2$RuO$_4$

The characteristic excitation of a metal is its plasmon, which is a quantized collective oscillation of its electron density. In 1956, David Pines predicted that a distinct type of plasmon, dubbed a "demon," could exist in three-dimensional metals containing more than one species of charge carrier. Consisting of out-of-phase movement of electrons in different bands, demons are acoustic, electrically neutral, and do not couple to light, so have never been detected in an equilibrium, three-dimensional metal. Nevertheless, demons are believed to be critical for diverse phenomena including phase transitions in mixed-valence semimetals, optical properties of metal nanoparticles, "soundarons" in Weyl semimetals, and high temperature superconductivity in, for example, metal hydrides. Here, we present evidence for a demon in Sr$_2$RuO$_4$ from momentum-resolved electron energy-loss spectroscopy (M-EELS). Formed of electrons in the $\beta$ and $\gamma$ bands, the demon is gapless with a room temperature velocity $v=1.065 \pm 0.12 \times 10^5$ m/s and critical momentum $q_c=0.08$ reciprocal lattice units. Its spectral weight violates low-energy partial sum rules, affirming its neutral character. Our study confirms a 66-year old prediction and suggests that demons may be a pervasive feature of multiband metals.

cond-mat.str-el↗

arXiv2019

Enhanced electron-phonon coupling for charge-density-wave formation in La$_{1.8-x}$Eu$_{0.2}$Sr$_{x}$CuO$_{4+\delta}$

Charge density wave (CDW) correlations are prevalent in all copper-oxide superconductors. While CDWs in conventional metals are driven by coupling between lattice vibrations and electrons, the role of the electron-phonon coupling (EPC) in cuprate CDWs is strongly debated. Using Cu $L_3$ edge resonant inelastic x-ray scattering (RIXS), we study the CDW and Cu-O bond-stretching phonons in the stripe-ordered cuprate La$_{1.8-x}$Eu$_{0.2}$Sr$_{x}$CuO$_{4+\delta}$. We investigate the interplay between charge order and EPC as a function of doping and temperature, and find that the EPC is enhanced in a narrow momentum region around the CDW wave vector. By detuning the incident photon energy from the absorption resonance, we extract an EPC matrix element at the CDW wave vector of $M\simeq$ 0.36 eV, which decreases to $M\simeq$ 0.30 eV at high temperature in the absence of the CDW. Our results suggest a feedback mechanism in which the CDW enhances the EPC which, in turn, further stabilizes the CDW.

cond-mat.supr-con↗

arXiv2019

Crossover of Charge Fluctuations across the Strange Metal Phase Diagram

A normal metal exhibits a valence plasmon, which is a sound wave in its conduction electron density. The mysterious strange metal is characterized by non-Boltzmann transport and violates most fundamental Fermi liquid scaling laws. A fundamental question is: Do strange metals have plasmons? Using momentum-resolved inelastic electron scattering (M-EELS) we recently showed that, rather than a plasmon, optimally-doped Bi$_{2.1}$Sr$_{1.9}$Ca$_{1.0}$Cu$_{2.0}$O$_{8+x}$ (Bi-2212) exhibits a featureless, temperature-independent continuum with a power-law form over most energy and momentum scales [M. Mitrano, PNAS 115, 5392-5396 (2018)]. Here, we show that this continuum is present throughout the fan-shaped, strange metal region of the phase diagram. Outside this region, dramatic changes in spectral weight are observed: In underdoped samples, spectral weight up to 0.5 eV is enhanced at low temperature, biasing the system towards a charge order instability. The situation is reversed in the overdoped case, where spectral weight is strongly suppressed at low temperature, increasing quasiparticle coherence in this regime. Optimal doping corresponds to the boundary between these two opposite behaviors at which the response is temperature-independent. Our study suggests that plasmons do not exist as well-defined excitations in Bi-2212, and that a featureless continuum is a defining property of the strange metal, which is connected to a peculiar crossover where the spectral weight change undergoes a sign reversal.

cond-mat.str-el↗

arXiv2018

Emergent Dirac carriers across a pressure-induced Lifshitz transition in black phosphorus

The phase diagrams of correlated systems like cuprates or pnictides high-temperature superconductors are characterized by a topological change of the Fermi surface under continuous variation of an external parameter, the so-called Lifshitz transition. However, the large number of low-temperature instabilities and the interplay of multiple energy scales complicate the study of this phenomenon. Here we first identify the optical signatures of a pressure-induced Lifshitz transition in a clean elemental system, black phosphorus. By applying external pressures above 1.5 GPa, we observe a change in the pressure dependence of the Drude plasma frequency due to the appearance of massless Dirac fermions. At higher pressures, optical signatures of two structural phase transitions are also identified. Our findings suggest that a key fingerprint of the Lifshitz transition in solid state systems, and in absence of structural phase transitions, is a discontinuity of the Drude plasma frequency due to the change of Fermi surface topology.

cond-mat.mtrl-sci↗

arXiv2017

Anomalous density fluctuations in a strange metal

A central mystery in high temperature superconductivity is the origin of the so-called "strange metal," i.e., the anomalous conductor from which superconductivity emerges at low temperature. Measuring the dynamic charge response of the copper-oxides, $\chi''(q,\omega)$, would directly reveal the collective properties of the strange metal, but it has never been possible to measure this quantity with meV resolution. Here, we present the first measurement of $\chi''(q,\omega)$ for a cuprate, optimally doped Bi$_2$Sr$_2$CaCu$_2$O$_{8+x}$ ($T_c=91$ K), using momentum-resolved inelastic electron scattering. In the medium energy range 0.1-2 eV relevant to the strange metal, the spectra are dominated by a featureless, temperature- and momentum-independent continuum persisting to the eV energy scale. This continuum displays a simple power law form, exhibiting $q^2$ behavior at low energy and $q^2/\omega^2$ behavior at high energy. Measurements of an overdoped crystal ($T_c=50$ K) showed the emergence of a gap-like feature at low temperature, indicating deviation from power law form outside the strange metal regime. Our study suggests the strange metal exhibits a new type of charge dynamics in which excitations are local to such a degree that space and time axes are decoupled.

cond-mat.str-el↗

arXiv2017

Pressure tuning of light-induced superconductivity in K3C60

Optical excitation at terahertz frequencies has emerged as an effective means to manipulate complex solids dynamically. In the molecular solid K3C60, coherent excitation of intramolecular vibrations was shown to transform the high temperature metal into a non-equilibrium state with the optical conductivity of a superconductor. Here we tune this effect with hydrostatic pressure, and we find it to disappear around 0.3 GPa. Reduction with pressure underscores the similarity with the equilibrium superconducting phase of K3C60, in which a larger electronic bandwidth is detrimental for pairing. Crucially, our observation excludes alternative interpretations based on a high-mobility metallic phase. The pressure dependence also suggests that transient, incipient superconductivity occurs far above the 150 K hypothesised previously, and rather extends all the way to room temperature.

cond-mat.supr-con↗