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Giacomo Merzoni

Publications and source records attributed to Giacomo Merzoni.

12 recordsLinked to original sources

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

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

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$_{7-δ}$ 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

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

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

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

Ultrafast decoupling of polarization and strain in ferroelectric BaTiO$_3$

A fundamental understanding of the interplay between lattice structure, polarization and electrons is pivotal to the optical control of ferroelectrics. The interaction between light and matter enables the remote and wireless control of the ferroelectric polarization on the picosecond timescale, while inducing strain, i.e., lattice deformation. At equilibrium, the ferroelectric polarization is proportional to the strain, and is typically assumed to be so also out of equilibrium. Decoupling the polarization from the strain would remove the constraint of sample design and provide an effective knob to manipulate the polarization by light. Here, upon an above-bandgap laser excitation of the prototypical ferroelectric BaTiO$_3$, we induce and measure an ultrafast decoupling between polarization and strain that begins within 350 fs, by softening Ti-O bonds via charge transfer, and lasts for several tens of picoseconds. We show that the ferroelectric polarization out of equilibrium is mainly determined by photoexcited electrons, instead of the strain. This excited state could serve as a starting point to achieve stable and reversible polarization switching via THz light. Our results demonstrate a light-induced transient and reversible control of the ferroelectric polarization and offer a pathway to control by light both electric and magnetic degrees of freedom in multiferroics.

cond-mat.mtrl-sci

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

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

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

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

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