arXiv subjects

Giacomo Ghiringhelli

Publications and source records attributed to Giacomo Ghiringhelli.

At least 19 recordsLinked to original sources

arXiv2026

Machine-learning test of the single-ion model for $dd$ excitations in cuprates

We investigate $dd$ excitations in Resonant Inelastic X-ray Scattering spectra of YBa$_2$Cu$_3$O$_6$ and La$_2$CuO$_4$ using the local single-ion model. The data are analyzed by conventional global fitting and by a convolutional neural network trained within the same theoretical framework. For YBa$_2$Cu$_3$O$_6$, the excited state energies obtained with the two methods coincide, leading to the $xy$, $3z^2-r^2$, $xz/yz$ sequence for increasing energy. This result validates the use of machine learning tools for the analysis of RIXS spectra dominated by $dd$ excitations. By contrast, for La$_2$CuO$_4$, the two methods do not converge to a single solution, revealing the limitations of the single-ion model in describing $dd$ excitations in cuprates and pointing to the role of additional contributions beyond a purely local picture in shaping high-energy excitations.

cond-mat.str-el↗

arXiv2026

Unveiling the Interplay of Charge and Magnetic Excitations in HgBa$_2$Ca$_2$Cu$_3$O$_{8+\delta}$

Unraveling the mechanism that binds electrons into Cooper pairs in cuprate high-temperature superconductors remains one of the most fundamental challenges in condensed-matter physics. While both magnetic interactions and lattice vibrations are known to govern key electronic properties, their possible cooperation has never been directly observed. We investigate HgBa$_2$Ca$_2$Cu$_3$O$_{8+\delta}$ (Hg1223) - the cuprate with the highest $T_{\mathrm{c}}$ at ambient pressure - as a magnifying glass to probe the possible entwining of the excitations at the core of the pairing. Using resonant inelastic X-ray scattering, we find that the charge response is dominated by dynamic charge density fluctuations (CDF) extending up to several hundred meV, where magnetic excitations reside. At the same momentum where CDF are most intense, the paramagnon energy exhibits a pronounced softening, revealing a strong interplay among charge, lattice, and spin excitations. Our results point to a cooperative mechanism in which dynamic charge fluctuations mediate the coupling between lattice, charge and spin degrees of freedom-shedding new light on the fundamental origin of high-$T_{\mathrm{c}}$ superconductivity.

cond-mat.supr-con↗

arXiv2026

Ultrafast Two-Dimensional Spectroscopy Uncovers Ubiquitous Electron-Paramagnon Coupling in Cuprate Superconductors

The coupling between electronic excitations and collective bosonic modes is fundamental to the emergence of high-temperature superconductivity in cuprates. Despite extensive effort, conventional equilibrium and pump-probe optical spectroscopies still struggle to disentangle couplings to different bosonic modes when their energy scales overlap. Here we overcome this limitation using ultrafast two-dimensional electronic spectroscopy (2DES), which correlates coherent excitation and detection photon energies with femtosecond time resolution. Applied to optimally doped Bi$_2$Sr$_2$Ca$_{0.92}$Y$_{0.08}$Cu$_2$O$_{8+\delta}$, 2DES reveals a pronounced off-diagonal resonance arising from the ultrafast generation of non-thermal bosons with energy $\hbar\Omega_\mathbf{q}\simeq200$ meV. By comparing the measured spectra with a theoretical framework that explicitly includes the interaction between charge-transfer and magnetic excitations, we identify these bosons as paramagnons with momenta centered near $(\pi/2,\pi/2)$ and extending toward $(0,\pi)$ and $(\pi,0)$. The resonance persists across a large range of temperatures and doping concentrations, demonstrating that high-energy paramagnons are ubiquitously and strongly coupled to electronic excitations throughout the cuprate phase diagram. Time-domain analysis constrains the build-up of the paramagnon population to $\lesssim 10$ fs, placing a lower bound $\lambda \gtrsim 0.7$ on the coupling strength. More broadly, our results establish 2DES as a powerful approach for disentangling mode-selective electron-boson interactions and addressing decoherence dynamics, thereby establishing a new avenue for investigating strongly correlated quantum materials. These findings also provide a direct framework for future time-resolved resonant inelastic X-ray scattering experiments aimed at tracking the ultrafast dynamics of magnetic excitations.

cond-mat.supr-con↗

arXiv2026

Electron-phonon coupling revealed by charge density fluctuations in cuprate superconductors

Electron-phonon coupling (EPC) governs lattice dynamics, charge transport, and collective electronic phases in quantum materials. In several families of unconventional superconductors, including transition-metal dichalcogenides and kagome metals, growing evidence points to a cooperative role of EPC and dynamic charge-density fluctuations (CDF) in stabilizing superconductivity. However, how the EPC strength evolves across phase diagrams and relates to superconducting properties in strongly correlated systems remains an open question. Here we investigate the interplay between phonons and the CDF recently identified in cuprate superconductors. Using resonant inelastic x-ray scattering, we track the dispersion and intensity of bond-stretching phonons in YBa$_2$Cu$_3$O$_{7-\delta}$ over wide ranges of doping, temperature, and momentum. We find that both the phonon softening at the CDF wave vector and the EPC strength, extracted from a pronounced phonon intensity anomaly, are maximized near $p = 0.19$, where superconducting properties are optimal and CDF intensity is strongest. These results identify dynamic charge-density fluctuations, rather than quasi-static charge density waves, as the dominant source of phonon renormalization in cuprates, and establish a direct correlation between EPC strength and the superconducting dome. More broadly, our measurements highlight EPC as a doping-dependent property of correlated materials, shaped by the electronic environment in which lattice vibrations are embedded.

cond-mat.supr-con↗

arXiv2025

Evaluating covalency using RIXS spectral weights: Silver fluorides vs. cuprates

We investigate the electronic structure of AgF2, AgFBF4, AgF and Ag2O using X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS) at the Ag L3 edge. XAS results were compared with density functional theory computations of the spectra, allowing an identification of main features and an assessment of the theoretical approximations. Our RIXS measurements reveal that AgF2 exhibits charge transfer excitations and dd excitations, analogous to those observed in La2CuO4. We propose to use the ratio of dd to CT spectral weight as a measure of the covalence of the compounds and provide explicit equations for the weights as a function of the scattering geometry for crystals and powders. The measurements at the metal site L3 edge and previous measurements at the ligand K edge reveal a striking similarity between the fluorides and cuprates materials, with fluorides somewhat more covalent than cuprates. These findings support the hypothesis that silver fluorides are an excellent platform to mimic the physics of cuprates, providing a promising avenue for exploring high-Tc superconductivity and exotic magnetism in quasi-two-dimensional (AgF2) and quasi-one-dimensional (AgFBF4) materials.

cond-mat.str-el↗

arXiv2025

Collective Magnetic Excitations in a Photo-excited Electron-doped Cuprate Superconductor

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.

cond-mat.mtrl-sci↗

arXiv2025

Spin and orbital excitations in undoped infinite layers: a comparison between superconducting PrNiO2 and insulating CaCuO2

Infinite-layer nickelates are among the most promising cuprate-akin superconductors, although relevant differences from copper oxides have been reported. Here, we present momentum- and polarization-resolved RIXS measurements on chemically undoped, superconducting PrNiO2, and compare its magnetic and orbital excitations with those of the reference infinite layer cuprate CaCuO2. In PrNiO2, the in-plane magnetic exchange integrals are smaller than in CaCuO2, whereas the out-of-plane values are similar, indicating that both materials support a three-dimensional antiferromagnetic order. Orbital excitations, associated to the transitions within 3d states of the metal, are well reproduced within a single-ion model and display similar characteristics, except for the Ni-dxy peak which, besides lying at significantly lower energy, shows an opposite dispersion to that of Cu-dxy. This is interpreted as a consequence of orbital superexchange coupling between nearest neighbor sites, which drives the orbiton propagation. Our observations demonstrate that infinite layer cuprates and nickelates share most of the spin and orbital properties, despite their markedly different charge-transfer energy Delta.

cond-mat.supr-con↗

arXiv2025

X-raying Mg0.2Co0.2Ni0.2Cu0.2Zn0.2O: disentangling elemental contributions in a prototypical high-entropy oxide

We employ several X-ray based techniques, including X-ray diffraction, absorption and resonant inelastic scattering, to disentangle the contributions of individual chemical species to the structural, electronic and magnetic properties of high-entropy oxides. In the benchmark compound Mg0.2Co0.2Ni0.2Cu0.2Zn0.2O and related systems, we unambiguously resolve a sizable Jahn-Teller distortion at the Cu sites, more pronounced in the absence of Ni2+ and Mg2+, suggesting that these ions promote positional order, whereas Cu2+ ions act to destabilize it. Moreover, we detect magnetic excitations and estimate the strength of the interactions between pairs of different magnetic elements. Our results provide valuable insights into the role of the various chemical species in shaping the physical properties of high-entropy oxides.

cond-mat.mtrl-sci↗

arXiv2025

Photo-generated charge-transfer excitons in NiO revealed by ultrafast time-resolved resonant inelastic x-ray scattering

Strong electronic correlation can lead to insulating behavior and to the opening of large optical gaps, even in materials with partly filled valence shells. Although the non-equilibrium optical response encodes both local (quasi atomic) and collective (long range) responses, optical spectroscopy is usually more sensitive to the latter. Resonant x-ray techniques are better suited to investigate the quasi-atomic properties of correlated solids. Using time-resolved resonant inelastic x-ray scattering (RIXS), here we study the ultrafast non-equilibrium processes in NiO following photo-excitation by ultraviolet photons with energy exceeding the optical gap. We observe the creation of charge-transfer excitons that decay with a time constant of about 2\,ps, while itinerant photo-doping persists for tens of picoseconds. Following our discovery, which establishes time-resolved high-resolution RIXS as a powerful tool for the study of transient phenomena in condensed matter, the possible presence of charge-transfer excitons will need to be considered when interpreting optical pump-probe experiments on correlated quantum materials.

cond-mat.str-el↗

arXiv2025

The influence of phonon symmetry and electronic structure on the electron-phonon coupling momentum dependence in cuprates

The experimental determination of the magnitude and momentum dependence of electron-phonon coupling (EPC) is an outstanding problem in condensed matter physics. The intensity of phonon peaks in Resonant Inelastic X-ray Scattering (RIXS) spectra can be related to the underlying EPC strength under significant approximations whose validity deserves careful verification. We measured the Cu L$_3$ RIXS phonon intensity as function of incident photon energy and of momentum transfer in several layered cuprates. For CaCuO$_2$, La$_{2-x}$Sr$_{x}$CuO$_{4+\delta}$, and \ch{YBa_2Cu_3O_{6}}, using a generally accepted theoretical model, we estimate quantitatively the EPC for the bond-stretching mode along the high-symmetry directions ($\zeta$,0) and ($\zeta$,$\zeta$), and as a function of the azimuthal angle $\varphi$ at fixed $q_\parallel$. We compare our results with theoretical predictions and we find that the $\mathbf{q}_\parallel$-dependence of the phonon RIXS intensity can be largely ascribed to the phonon symmetry. However, a more satisfactory prediction of the experimental results requires an accurate description of the electronic structure close to the Fermi level. Our extensive investigation indicates that Cu L$_3$ RIXS can be reliably used to determine the momentum dependence of EPC for the bond-stretching modes of cuprates. Moreover, the large experimental basis provided in this article can serve as stringent test for advanced theoretical predictions on the EPC.

cond-mat.str-el↗

arXiv2024

Superconductivity in PrNiO2 infinite-layer nickelates

Several reports about infinite-layer nickelate thin films suggest that the superconducting critical temperature versus chemical doping phase diagram has a dome-like shape, similar to cuprates. Here, we demonstrate a highly reproducible superconducting state in undoped PrNiO$_2$ thin films grown onto SrTiO$_3$. Scanning transmission electron microscopy measurements demonstrate coherent and defect-free infinite-layer phase, a high structural quality with no unintentional chemical doping and a total absence of interstitial oxygen. X-ray absorption measurements show very sharp features at the Ni L$_{3,2}$-edges with a large linear dichroism, indicating the preferential hole-occupation of Ni$^{1+}$-3d$_{x^2-y^2}$ orbitals in a square planar geometry. Resonant inelastic X-ray scattering measurements reveal sharp magnon excitations of 200\,meV energy at magnetic Brillouin zone boundary, highly resonant at the Ni$^{1+}$ absorption peak. The results indicate that, when properly stabilized, infinite-layer nickelate thin films are superconducting without chemical doping.

cond-mat.supr-con↗

arXiv2024

Spin excitations in Nd1-xSrxNiO2 and YBa2Cu3O7-delta: the influence of Hubbard U

We use Resonant Inelastic X-ray Scattering (RIXS) to compare the doping dependence of magnetic excitations of an Infinite-Layer nickelate to those of a prototypical superconducting cuprate. The polarization analysis of RIXS spectra establishes the dominant spin-flip nature of the mid-infrared peak in both cases. Hole doping leads to opposite behavior of the magnetic energy in the two materials. By fitting the data with an original Hubbard-based model for dynamic susceptibility, we find that t is comparable in the two materials while U is about twice larger in the nickelate. This finding accounts for the smaller magnetic bandwidth of nickelates and for its decrease upon doping.

cond-mat.str-el↗

arXiv2024

Charge response function probed by resonant inelastic x-ray scattering: the signature of electronic gaps of YBa$_2$Cu$_3$O$_{7-δ}$

In strongly correlated systems the complete determination of the dynamical susceptibility $χ(\textbf{q}, ω)$ is of special relevance because of the entwinement of the spin and charge components. Although Resonant Inelastic X-Ray Scattering (RIXS) spectra are directly related to both the charge ($χ''_c(\textbf{q}, ω)$) and the spin ($χ''_s(\textbf{q}, ω)$) contributions, only the latter has been extensively studied with RIXS so far. Here we show how to extract from RIXS spectra of high-$T_c$ superconducting cuprates relevant properties of $χ''_c$, such as the presence of the superconducting gap and of the pseudogap. In particular, we exploit the temperature dependence of the Cu L$_3$ edge RIXS spectra of underdoped YBa$_2$Cu$_3$O$_{7-δ}$ at specific wave-vectors q. The signature of the two gaps is in the departure of the low energy Bosonic excitation continuum from the statistical temperature-dependence. This approach can be immediately used to investigate systematically the nature of the pseudogap in cuprates, thereby taking advantage of the RIXS technique that does not suffer the limitations of surface-sensitive electron spectroscopies. Its extension to other interesting materials is foreseen.

cond-mat.supr-con↗

arXiv2024

The Heisenberg-RIXS instrument at the European XFEL

Resonant Inelastic X-ray Scattering (RIXS) is an ideal X-ray spectroscopy method to push the combination of energy and time resolutions to the Fourier transform ultimate limit, because it is unaffected by the core-hole lifetime energy broadening. And in pump-probe experiments the interaction time is made very short by the same core-hole lifetime. RIXS is very photon hungry so it takes great advantage from high repetition rate pulsed X-ray sources like the European XFEL. The hRIXS instrument is designed for RIXS experiments in the soft X-ray range with energy resolution approaching the Fourier and the Heisenberg limits. It is based on a spherical grating with variable line spacing (VLS) and a position-sensitive 2D detector. Initially, two gratings are installed to adequately cover the whole photon energy range. With optimized spot size on the sample and small pixel detector the energy resolution can be better than 40 meV at any photon energy below 1000 eV. At the SCS instrument of the European XFEL the spectrometer can be easily positioned thanks to air-pads on a high-quality floor, allowing the scattering angle to be continuously adjusted over the 65-145 deg range. It can be coupled to two different sample interaction chamber, one for liquid jets and one for solids, each equipped at the state-of-the-art and compatible for optical laser pumping in collinear geometry. The measured performances, in terms of energy resolution and count rate on the detector, closely match design expectations. hRIXS is open to public users since the summer of 2022.

cond-mat.str-el↗

arXiv2024

Collective nature of orbital excitations in layered cuprates in the absence of apical oxygens

We have investigated the 3d orbital excitations in CaCuO2 (CCO), Nd2CuO4 (NCO), and La2CuO4 (LCO) using high-resolution resonant inelastic x-ray scattering. In LCO they behave as well-localized excitations, similarly to several other cuprates. On the contrary, in CCO and NCO the dxy orbital clearly disperse, pointing to a collective character of this excitation (orbiton) in compounds without apical oxygen. We ascribe the origin of the dispersion as stemming from a substantial next-nearest-neighbor (NNN) orbital superexchange. Such an exchange leads to the liberation of orbiton from its coupling to magnons, which is associated with the orbiton hopping between nearest neighbor copper sites. We show that the exceptionally large NNN orbital superexchange can be traced back to the absence of apical oxygens suppressing the charge transfer energy.

cond-mat.str-el↗

arXiv2023

Absence of localized $5d^1$ electrons in KTaO$_3$ interface superconductors

Recently, an exciting discovery of orientation-dependent superconductivity was made in two-dimensional electron gas (2DEG) at the interfaces of LaAlO$_3$/KTaO$_3$ (LAO/KTO) or EuO/KTaO$_3$ (EuO/KTO). The superconducting transition temperature can reach a $T_c$ of up to $\sim$ 2.2 K, which is significantly higher than its 3$d$ counterpart LaAlO$_3$/SrTiO$_3$ (LAO/STO) with a $T_c$ of $\sim$ 0.2 K. However, the underlying origin remains to be understood. To uncover the nature of electrons in KTO-based interfaces, we employ x-ray absorption spectroscopy (XAS) and resonant inelastic x-ray spectroscopy (RIXS) to study LAO/KTO and EuO/KTO with different orientations. We reveal the absence of $dd$ orbital excitations in all the measured samples. Our RIXS results are well reproduced by calculations that considered itinerant $5d$ electrons hybridized with O $2p$ electrons. This suggests that there is a lack of localized Ta $5d^1$ electrons in KTO interface superconductors, which is consistent with the absence of magnetic hysteresis observed in magneto-resistance (MR) measurements. These findings offer new insights into our understanding of superconductivity in Ta $5d$ interface superconductors and their potential applications.

cond-mat.supr-con↗

arXiv2022

Identification of a Critical Doping for Charge Order Phenomena in Bi-2212 Cuprates via RIXS

Identifying quantum critical points (QCPs) and their associated fluctuations may hold the key to unraveling the unusual electronic phenomena observed in cuprate superconductors. Recently, signatures of quantum fluctuations associated with charge order (CO) have been inferred from the anomalous enhancement of CO excitations that accompany the reduction of the CO order parameter in the superconducting state. To gain more insight about the interplay between CO and superconductivity, here we investigate the doping dependence of this phenomenon throughout the Bi-2212 cuprate phase diagram using resonant inelastic x-ray scattering (RIXS) at the Cu L3- edge. As doping increases, the CO wavevector decreases, saturating at a commensurate value of 0.25 r.l.u. beyond a characteristic doping pc, where the correlation length becomes shorter than the apparent periodicity (4a0). Such behavior is indicative of the fluctuating nature of the CO; and the proliferation of CO excitations in the superconducting state also appears strongest at pc, consistent with expected behavior at a CO QCP. Intriguingly, pc appears to be near optimal doping, where the superconducting transition temperature Tc is maximal.

cond-mat.supr-con↗

arXiv2022

Charge Transfer and $dd$ excitations in AgF$_{2}$

Charge transfer (CT) insulators are the parent phase of a large group of today's unconventional high-temperature superconductors. Here we study experimentally and theoretically the interband excitations of the CT insulator silver fluoride AgF$_2$, which has been proposed as an excellent analogue of oxocuprates. Optical conductivity and resonant inelastic X-ray scattering (RIXS) on AgF$_2$ polycrystalline sample show a close similarity with that measured on undoped La$_2$CuO$_4$. While the former shows a CT gap $\sim$3.4 eV, larger than in the cuprate, $dd$ excitations are nearly at the same energy in the two materials. DFT and exact diagonalization cluster computations of the multiplet spectra show that AgF$_2$ is more covalent than the cuprate, in spite of the larger fundamental gap. Furthermore, we show that AgF$_2$ is at the verge of a charge transfer instability. The overall resemblance of our data on AgF$_2$ to those published previously on La$_2$CuO$_4$ suggests that the underlying CT insulator physics is the same, while AgF$_2$ could also benefit from a proximity to a charge density wave phase as in BaBiO$_3$. Therefore, our work provides a compelling support to the future use of fluoroargentates for materials' engineering of novel high-temperature superconductors.

cond-mat.supr-con↗