arXiv subjects

Leonardo Martinelli

Publications and source records attributed to Leonardo Martinelli.

16 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

Direct High-Magnetic-Field Coupling to Stripe Order in a Cuprate Superconductor

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.

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

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

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

Weak-signal extraction enabled by deep-neural-network denoising of diffraction data

Removal or cancellation of noise has wide-spread applications for imaging and acoustics. In every-day-life applications, denoising may even include generative aspects, which are unfaithful to the ground truth. For scientific use, however, denoising must reproduce the ground truth accurately. Here, we show how data can be denoised via a deep convolutional neural network such that weak signals appear with quantitative accuracy. In particular, we study X-ray diffraction on crystalline materials. We demonstrate that weak signals stemming from charge ordering, insignificant in the noisy data, become visible and accurate in the denoised data. This success is enabled by supervised training of a deep neural network with pairs of measured low- and high-noise data. We demonstrate that using artificial noise does not yield such quantitatively accurate results. Our approach thus illustrates a practical strategy for noise filtering that can be applied to challenging acquisition problems.

eess.IV↗

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↗

arXiv2021

Doping-dependence of the electron-phonon coupling in two families of bilayer superconducting cuprates

While electron-phonon coupling (EPC) is crucial for Cooper pairing in conventional superconductors, its role in high-$T_c$ superconducting cuprates is debated. Using resonant inelastic x-ray scattering at the oxygen $K$-edge, we studied the EPC in Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ (Bi2212) and Nd$_{1+x}$Ba$_{2-x}$Cu$_3$O$_{7-δ}$ (NBCO) at different doping levels ranging from heavily underdoped ($p =0.07$) to overdoped ($p=0.21$). We analyze the data with a localized Lang-Firsov model that allows for the coherent excitations of two phonon modes. While electronic band dispersion effects are non-negligible, we are able to perform a study of the relative values of EPC matrix elements in these cuprate families. In the case of NBCO, the choice of the excitation energy allows us to disentangle modes related to the CuO$_3$ chains and the CuO$_2$ planes. Combining the results from the two families, we find the EPC strength decreases with doping at $\mathbf{q_\parallel}=(-0.25, 0)$ r.l.u., but has a non-monotonic trend as a function of doping at smaller momenta. This behavior is attributed to the screening effect of charge carriers. We also find that the phonon intensity is enhanced in the vicinity of the charge-density-wave (CDW) excitations while the extracted EPC strength appears to be less sensitive to their proximity. By performing a comparative study of two cuprate families, we are able to identify general trends in the EPC for the cuprates and provide experimental input to theories invoking a synergistic role for this interaction in $d$-wave pairing.

cond-mat.supr-con↗

arXiv2021

Fractional spin excitations in the infinite-layer cuprate CaCuO$_2$

We use resonant inelastic x-ray scattering (RIXS) to investigate the magnetic dynamics of the infinite-layer cuprate CaCuO2. We find that close to the (1/2,0) point the single magnon decays into a broad continuum of excitations accounting for 80% of the total magnetic spectral weight. Polarization resolved RIXS spectra reveal the overwhelming dominance of spin-flip ($ΔS = 1$) characterof this continuum with respect to the $ΔS= 0$ multimagnon contributions. Moreover, its incident energy dependence is identical to that of the magnon, supporting a common physical origin. We propose that the continuum originates from the decay of the magnon into spinon pairs, and we relate it to the exceptionally high ring exchange $J_\mathrm{c} \sim J_1$ of CaCuO2. In the infinite layer cuprates long-range and multi-site hopping integrals are pivotal and amplify the 2D quantum magnetism effects in spite the 3D antiferromagnetic Néel order.

cond-mat.str-el↗

arXiv2021

Multiple-magnon excitations shape the spin spectrum of cuprate parent compounds

Thanks to high resolution and polarization analysis, resonant inelastic x-ray scattering (RIXS) magnetic spectra of La2CuO4, Sr2CuO2Cl2 and CaCuO2 reveal a rich set of properties of the spin 1/2 antiferromagnetic square lattice of cuprates. The leading single-magnon peak energy dispersion is in excellent agreement with the corresponding inelastic neutron scattering measurements. However, the RIXS data unveil an asymmetric lineshape possibly due to odd higher order terms. Moreover, a sharp bimagnon feature emerges from the continuum at (1/2,0), coincident in energy with the bimagnon peak detected in optical spectroscopy. These findings show that the inherently complex spin spectra of cuprates, an exquisite manifestation of quantum magnetism, can be effectively explored by exploiting the richness of RIXS cross sections.

cond-mat.supr-con↗