arXiv subjects

Valentina Bisogni

Publications and source records attributed to Valentina Bisogni.

At least 37 records · Page 2Linked to original sources

arXiv2024

Elementary excitations of single-photon emitters in hexagonal Boron Nitride

Single-photon emitters serve as building blocks for many emerging concepts in quantum photonics. The recent identification of bright, tunable, and stable emitters in hexagonal boron nitride (hBN) has opened the door to quantum platforms operating across the infrared to ultraviolet spectrum. While it is widely acknowledged that defects are responsible for single-photon emitters in hBN, crucial details regarding their origin, electronic levels, and orbital involvement remain unknown. Here, we employ a combination of resonant inelastic X-ray scattering and photoluminescence spectroscopy in defective hBN unveiling an elementary excitation at 285 meV that gives rise to a plethora of harmonics correlated with single-photon emitters. We discuss the importance of N $π^*$ antibonding orbitals in shaping the electronic states of the emitters. The discovery of the elementary excitations of hBN provides new fundamental insights into quantum emission in low-dimensional materials, paving the way for future investigations in other platforms.

cond-mat.mes-hall↗

arXiv2023

Single- and Multimagnon Dynamics in Antiferromagnetic $α$-Fe$_2$O$_3$ Thin Films

Understanding the spin dynamics in antiferromagnetic (AFM) thin films is fundamental for designing novel devices based on AFM magnon transport. Here, we study the magnon dynamics in thin films of AFM $S=5/2$ $α$-Fe$_2$O$_3$ by combining resonant inelastic x-ray scattering, Anderson impurity model plus dynamical mean-field theory, and Heisenberg spin model. Below 100 meV, we observe the thickness-independent (down to 15 nm) acoustic single-magnon mode. At higher energies (100-500 meV), an unexpected sequence of equally spaced, optical modes is resolved and ascribed to $ΔS_z = 1$, 2, 3, 4, and 5 magnetic excitations corresponding to multiple, noninteracting magnons. Our study unveils the energy, character, and momentum-dependence of single and multimagnons in $α$-Fe$_2$O$_3$ thin films, with impact on AFM magnon transport and its related phenomena. From a broader perspective, we generalize the use of L-edge resonant inelastic x-ray scattering as a multispin-excitation probe up to $ΔS_z = 2S$. Our analysis identifies the spin-orbital mixing in the valence shell as the key element for accessing excitations beyond $ΔS_z = 1$, and up to, e.g., $ΔS_z = 5$. At the same time, we elucidate the novel origin of the spin excitations beyond the $ΔS_z = 2$, emphasizing the key role played by the crystal lattice as a reservoir of angular momentum that complements the quanta carried by the absorbed and emitted photons.

cond-mat.str-el↗

arXiv2022

Magnetic Excitations in Strained Infinite-layer Nickelate PrNiO2

Strongly correlated materials often respond sensitively to the external perturbations. In the recently discovered superconducting infinite-layer nickelates, the superconducting transition temperature can be dramatically enhanced via only ~1% compressive strain-tuning enabled by substrate design. However, the root of such enhancement remains elusive. While the superconducting pairing mechanism is still not settled, magnetic Cooper pairing - similar to the cuprates has been proposed. Using resonant inelastic x-ray scattering, we investigate the magnetic excitations in infinite-layer PrNiO2 thin films for different strain conditions. The magnon bandwidth of PrNiO2 shows only marginal response to strain-tuning, in sharp contrast to the striking enhancement of the superconducting transition temperature Tc in the doped superconducting samples. These results suggest the enhancement of Tc is not mediated by spin excitations and thus provide important empirics for the understanding of superconductivity in infinite-layer nickelates.

cond-mat.supr-con↗

arXiv2022

Strain-modulated anisotropic electronic structure in superconducting RuO$_2$ films

The binary ruthenate, RuO$_2$, has been the subject of intense interest due to its itinerant antiferromagnetism and strain-induced superconductivity. The strain mechanism and its effect on the microscopic electronic states leading to the normal and superconducting state, however, remain undisclosed. Here, we investigate highly-strained epitaxial (110) RuO$_2$ films using polarization-dependent oxygen K-edge X-ray absorption spectroscopy (XAS). Through the detection of pre-edge peaks, arising from O:$2p$ - Ru:$4d$ hybridization, we uncover the effects of epitaxial strain on the orbital/electronic structure near the Fermi level. Our data show robust strain-induced shifts of orbital levels and a reduction of hybridization strength. Furthermore, we reveal a pronounced in-plane anisotropy of the electronic structure along the $[110]/[1\bar{1}0]$ directions naturally stemming from the symmetry-breaking epitaxial strain of the substrate. The $B_{2g}$ symmetry component of the epitaxially-enforced strain breaks a sublattice degeneracy, resulting in an increase of the density of states at the Fermi level ($E_F$), possibly paving the way to superconductivity. These results underscore the importance of the effective reduction from tetragonal to orthorhombic lattice symmetry in (110) RuO$_2$ films and its relevance towards the superconducting and magnetic properties.

cond-mat.supr-con↗

arXiv2022

Site-specific electronic and magnetic excitations of the skyrmion material Cu$_2$OSeO$_3$

The manifestation of skyrmions in the Mott-insulator Cu$_2$OSeO$_3$ originates from a delicate balance between magnetic and electronic energy scales. As a result of these intertwined couplings, the two symmetry-inequivalent magnetic ions, Cu-I and Cu-II, bond into a spin S=1 entangled tetrahedron. However, conceptualizing the unconventional properties of this material and the energy of the competing interactions is a challenging task due the complexity of this system. Here we combine X-ray Absorption Spectroscopy and Resonant Inelastic X-ray Scattering to uncover the electronic and magnetic excitations of Cu$_2$OSeO$_3$ with site-specificity. We quantify the energies of the 3d crystal-field splitting for both Cu-I and Cu-II, fundamental to optimize model Hamiltonians. Additionally, we unveil a site-specific magnetic mode, indicating that individual spin character is preserved within the entangled-tetrahedron picture. Our results thus provide experimental constraint for validating theories that describe the interactions of Cu$_2$OSeO$_3$, highlighting the site-selective capabilities of resonant spectroscopies

cond-mat.str-el↗

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

High energy spin excitations in the quantum spin liquid candidate Zn-barlowite probed by resonant inelastic x-ray scattering

A quantum spin liquid is a novel ground state that can support long-range entanglement between magnetic moments, resulting in exotic spin excitations involving fractionalized $S=\frac{1}{2}$ spinons. Here, we measure the excitations in single crystals of the spin liquid candidate Zn-barlowite using resonant inelastic X-ray scattering. By analyzing the incident polarization and temperature dependences, we deduce a clear magnetic scattering contribution forming a broad continuum that surprisingly extends up to $\sim$200 meV ($\sim$14$J$, where $J$ is the magnetic exchange). The excitation spectrum reveals that significant contributions arise from multiple pairs of spinons and/or antispinons at high energies.

cond-mat.str-el↗

arXiv2021

Local electronic structure of rutile RuO$_2$

Recently, rutile RuO$_2$ has raised interest for its itinerant antiferromagnetism, crystal Hall effect, and strain-induced superconductivity. Understanding and manipulating these properties demands resolving the electronic structure and the relative roles of the rutile crystal field and $4d$ spin-orbit coupling (SOC). Here, we use O-K and Ru $M_3$ x-ray absorption (XAS) and Ru $M_3$ resonant inelastic x-ray scattering (RIXS) to disentangle the contributions of crystal field, SOC, and electronic correlations in RuO$_2$. The locally orthorhombic site symmetry of the Ru ions introduces significant crystal field contributions beyond the approximate octahedral coordination yielding a crystal field energy scale of $Δ(t_{2g})\approx 1$ eV breaking the degeneracy of the $t_{2g}$ orbitals. This splitting exceeds the Ru SOC ($\approx160$ meV) suggesting a more subtle role of SOC, primarily through the modification of itinerant (rather than local) $4d$ electronic states, ultimately highlighting the importance of the local symmetry in RuO$_2$. Remarkably, our analysis can be extended to other members of the rutile family, thus advancing the comprehension of the interplay among crystal field symmetry, electron correlations, and SOC in transition metal compounds with the rutile structure.

cond-mat.str-el↗

arXiv2020

Tuning spin excitations in magnetic films by confinement

Spin excitations of magnetic thin films are the founding element for novel transport concepts in spintronics, magnonics, and magnetic devices in general. While spin dynamics have been extensively studied in bulk materials, their behaviour in mesoscopic films is less known due to experimental limitations. Here, we employ Resonant Inelastic X-Ray Scattering to investigate the spin excitation spectrum in mesoscopic Fe films, from bulk-like down to 3 unit cells thick. In bulk-like samples, we find isotropic, dispersive ferromagnons consistent with the dispersion observed by neutron scattering in bulk single crystals. As the thickness is reduced, these ferromagnons survive and evolve anisotropically: renormalising to lower energies along the out-of-plane direction while retaining their dispersion in the in-plane direction. This thickness dependence is captured by simple Heisenberg model calculations accounting for the confinement in the out-of-plane direction through the loss of Fe bonds. Our findings highlight the effects of mesoscopic scaling on spin dynamics and identify thickness as a knob for fine-tuning and controlling magnetic properties in films.

cond-mat.str-el↗

arXiv2020

Microscopic Relaxation Channels in Materials for Superconducting Qubits

Despite mounting evidence that materials imperfections are a major obstacle to practical applications of superconducting qubits, connections between microscopic material properties and qubit coherence are poorly understood. Here, we perform measurements of transmon qubit relaxation times $T_1$ in parallel with spectroscopy and microscopy of the thin polycrystalline niobium films used in qubit fabrication. By comparing results for films deposited using three techniques, we reveal correlations between $T_1$ and grain size, enhanced oxygen diffusion along grain boundaries, and the concentration of suboxides near the surface. Physical mechanisms connect these microscopic properties to residual surface resistance and $T_1$ through losses arising from the grain boundaries and from defects in the suboxides. Further, experiments show that the residual resistance ratio can be used as a figure of merit for qubit lifetime. This comprehensive approach to understanding qubit decoherence charts a pathway for materials-driven improvements of superconducting qubit performance.

physics.app-ph↗

arXiv2019

Resonant inelastic x-ray scattering study of $α$-RuCl$_3$: a progress report

Ru M$_3$-edge resonant inelastic x-ray scattering (RIXS) measurements of RuCl$_3$ with 27 meV resolution reveals a spin-orbit exciton without noticeable splitting. We extract values for the spin-orbit coupling constant ($λ=154\pm2$ meV) and trigonal distortion field energy ($\left|Δ\right|<65$ meV) which support the $j_{\rm eff}=1/2$ nature of RuCl$_3$. We demonstrate the feasibility of M-edge RIXS for $4d$ systems, which allows ultra high-resolution RIXS of $4d$ systems until instrumentation for L-edge RIXS improves.

cond-mat.str-el↗

arXiv2017

Dispersive Magnetic and Electronic Excitations in Iridate Perovskites Probed with Oxygen $K$-Edge Resonant Inelastic X-ray Scattering

Resonant inelastic X-ray scattering (RIXS) experiments performed at the oxygen-$K$ edge on the iridate perovskites {\SIOS} and {\SION} reveal a sequence of well-defined dispersive modes over the energy range up to $\sim 0.8$ eV. The momentum dependence of these modes and their variation with the experimental geometry allows us to assign each of them to specific collective magnetic and/or electronic excitation processes, including single and bi-magnons, and spin-orbit and electron-hole excitons. We thus demonstrated that dispersive magnetic and electronic excitations are observable at the O-$K$ edge in the presence of the strong spin-orbit coupling in the $5d$ shell of iridium and strong hybridization between Ir $5d$ and O $2p$ orbitals, which confirm and expand theoretical expectations. More generally, our results establish the utility of O-$K$ edge RIXS for studying the collective excitations in a range of $5d$ materials that are attracting increasing attention due to their novel magnetic and electronic properties. Especially, the strong RIXS response at O-$K$ edge opens up the opportunity for investigating collective excitations in thin films and heterostructures fabricated from these materials.

cond-mat.str-el↗

arXiv2016

Orbital breathing effects in the computation of x-ray d-ion spectra in solids by ab initio wave-function-based methods

In existing theoretical approaches to core-level excitations of transition-metal ions in solids relaxation and polarization effects due to the inner core hole are often ignored or described phenomenologically. Here we set up an ab initio computational scheme that explicitly accounts for such physics in the calculation of x-ray absorption and resonant inelastic x-ray scattering spectra. Good agreement is found with experimental transition-metal $L$-edge data for the strongly correlated $d^9$ cuprate Li$_2$CuO$_2$, for which we determine the absolute scattering intensities. The newly developed methodology opens the way for the investigation of even more complex $d^n$ electronic structures of group VI B to VIII B correlated oxide compounds.

cond-mat.str-el↗

arXiv2016

Intra-layer doping effects on the high-energy magnetic correlations in NaFeAs

We have used Resonant Inelastic X-ray Scattering (RIXS) and dynamical susceptibility calculations to study the magnetic excitations in NaFe$_{1-x}$Co$_x$As (x = 0, 0.03, and 0.08). Despite a relatively low ordered magnetic moment, collective magnetic modes are observed in parent compounds (x = 0) and persist in optimally (x = 0.03) and overdoped (x = 0.08) samples. Their magnetic bandwidths are unaffected by doping within the range investigated. High energy magnetic excitations in iron pnictides are robust against doping, and present irrespectively of the ordered magnetic moment. Nevertheless, Co doping slightly reduces the overall magnetic spectral weight, differently from previous studies on hole-doped BaFe$_{2}$As$_{2}$, where it was observed constant. Finally, we demonstrate that the doping evolution of magnetic modes is different for the dopants being inside or outside the Fe-As layer.

cond-mat.supr-con↗

arXiv2016

Probing inter- and intrachain Zhang-Rice excitons in Li$_2$CuO$_2$ and determining their binding energy

Cuprate materials, like those hosting high temperature superconductivity, represent a famous class of materials where the correlations between the strongly entangled charges and spins produce complex phase diagrams. Several years ago the Zhang-Rice singlet was proposed as a natural quasiparticle in hole-doped cuprates. The occurance and binding energy of this quasiparticle, consisting of a pair of bound holes with antiparallel spins on the same CuO$_4$ plaquette, depends on the local electronic interactions, which are fundamental quantities for understanding the physics of the cuprates. Here, we employ state-of-the-art Resonant Inelastic X-ray Scattering (RIXS) to probe the correlated physics of the CuO$_4$ plaquettes in the quasi-one dimensional chain cuprate Li$_2$CuO$_2$. By tuning the incoming photon energy to the O $K$-edge, we populate bound states related to the Zhang-Rice quasiparticles in the RIXS process. Both intra- and interchain Zhang-Rice singlets are observed and their occurrence is shown to depend on the nearest-neighbor spin-spin correlations, which are readily probed in this experiment. We also extract the binding energy of the Zhang-Rice singlet and identify the Zhang-Rice triplet excitation in the RIXS spectra.

cond-mat.str-el↗

arXiv2016

Ground state oxygen holes and the metal-insulator transition in the negative charge transfer rare-earth nickelates

The metal-insulator transitions and the intriguing physical properties of rare-earth perovskite nickelates have attracted considerable attention in recent years. Nonetheless, a complete understanding of these materials remains elusive. Here, taking a NdNiO3 thin film as a representative example, we utilize a combination of x-ray absorption and resonant inelastic x-ray scattering (RIXS) spectroscopies to resolve important aspects of the complex electronic structure of the rare-earth nickelates. The unusual coexistence of bound and continuum excitations observed in the RIXS spectra provides strong evidence for the abundance of oxygen 2p holes in the ground state of these materials. Using cluster calculations and Anderson impurity model interpretation, we show that these distinct spectral signatures arise from a Ni 3d8 configuration along with holes in the oxygen 2p valence band, confirming suggestions that these materials do not obey a conventional positive charge-transfer picture, but instead exhibit a negative charge-transfer energy, in line with recent models interpreting the metal to insulator transition in terms of bond disproportionation.

cond-mat.str-el↗

arXiv2015

Electron-lattice interactions strongly renormalize the charge transfer energy in the spin-chain cuprate Li$_2$CuO$_2$

Strongly correlated insulators are broadly divided into two classes: Mott-Hubbard insulators, where the insulating gap is driven by the Coulomb repulsion $U$ on the transition-metal cation, and charge-transfer insulators, where the gap is driven by the charge transfer energy $Δ$ between the cation and the ligand anions. The relative magnitudes of $U$ and $Δ$ determine which class a material belongs to, and subsequently the nature of its low-energy excitations. These energy scales are typically understood through the local chemistry of the active ions. Here we show that the situation is more complex in the low-dimensional charge transfer insulator Li$_\mathrm{2}$CuO$_\mathrm{2}$, where $Δ$ has a large non-electronic component. Combining resonant inelastic x-ray scattering with detailed modeling, we determine how the elementary lattice, charge, spin, and orbital excitations are entangled in this material. This results in a large lattice-driven renormalization of $Δ$, which significantly reshapes the fundamental electronic properties of Li$_\mathrm{2}$CuO$_\mathrm{2}$.

cond-mat.str-el↗

arXiv2015

Orbital control of effective dimensionality: from spin-orbital fractionalization to confinement in the anisotropic ladder system CaCu2O3

Fractionalization of an electronic quasiparticle into spin, charge and orbital parts is a fundamental and characteristic property of interacting electrons in one dimension. However, real materials are never strictly one-dimensional and the fractionalization phenomena are hard to observe. Here we studied the spin and orbital excitations of the anisotropic ladder material CaCu2O3, whose electronic structure is not one-dimensional. Combining high-resolution resonant inelastic x-ray scattering experiments with theoretical model calculations we show that: (i) spin-orbital fractionalization occurs in CaCu2O3 along the leg direction x through the xz orbital channel as in a 1D system; and (ii) no fractionalization is observed for the xy orbital, which extends in both leg and rung direction, contrary to a 1D system. We conclude that the directional character of the orbital hopping can select different degrees of dimensionality. Using additional model calculations, we show that spin-orbital separation is generally far more robust than the spin-charge separation. This is not only due to the already mentioned selection realized by the orbital hopping, but also due to the fact that spinons are faster than the orbitons.

cond-mat.str-el↗