arXiv subjects

Jonathan Pelliciari

Publications and source records attributed to Jonathan Pelliciari.

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↗

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

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↗

arXiv2023

Stripe Symmetry of Short-range Charge Density Waves in Cuprate Superconductors

The omnipresence of charge density waves (CDWs) across almost all cuprate families underpins a common organizing principle. However, a longstanding debate of whether its spatial symmetry is stripe or checkerboard remains unresolved. While CDWs in lanthanum- and yttrium-based cuprates possess a stripe symmetry, distinguishing these two scenarios has been challenging for the short-range CDW in bismuth-based cuprates. Here, we employed high-resolution resonant inelastic x-ray scattering to uncover the spatial symmetry of the CDW in Bi$_2$Sr$_{2-x}$La$_{x}$CuO$_{6+δ}$. Across a wide range of doping and temperature, anisotropic CDW peaks with elliptical shapes were found in reciprocal space. Based on Fourier transform analysis of real-space models, we interpret the results as evidence of unidirectional charge stripes, hosted by mutually 90$^\circ$-rotated anisotropic domains. Our work paves the way for a unified symmetry and microscopic description of CDW order in cuprates.

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↗

arXiv2021

Fluctuating magnetism of Co- and Cu-doped NaFeAs

We report an x-ray emission spectroscopy (XES) study of the local fluctuating magnetic moment ($μ_{bare}$) in $\mathrm{NaFe_{1-x}Co_{x}As}$ and $\mathrm{NaFe_{1-x}Cu_{x}As}$. In NaFeAs, the reduced height of the As ions induces a local magnetic moment higher than $\mathrm{Ba_2As_2}$, despite lower T$_N$ and ordered magnetic moment. As NaFeAs is doped with Co $μ_{bare}$ is slightly reduced, whereas Cu doping leaves it unaffected, indicating a different doping mechanism: based on electron counting for Co whereas impurity scattering dominates in the case of Cu. Finally, we observe an increase of $μ_{bare}$ with temperature in all samples as observed in electron- and hole-doped $\mathrm{BaFe_2As_2}$. Since both Co and Cu doping display superconductivity, our findings demonstrate that the formation of Cooper pairs is not connected with the complete loss of fluctuating paramagnetic moments.

cond-mat.supr-con↗

arXiv2021

Spin dynamics in NaFeAs and NaFe$_{0.53}$Cu$_{0.47}$As probed by resonant inelastic X-ray scattering

The parent compounds of iron-based superconductors are magnetically-ordered bad metals, with superconductivity appearing near a putative magnetic quantum critical point. The presence of both Hubbard repulsion and Hund's coupling leads to rich physics in these multiorbital systems, and motivated descriptions of magnetism in terms of itinerant electrons or localized spins. The NaFe$_{1-x}$Cu$_x$As series consists of magnetically-ordered bad metal ($x=0$), superconducting ($x\approx0.02$) and magnetically-ordered semiconducing/insulating ($x\approx0.5$) phases, providing a platform to investigate the connection between superconductivity, magnetism and electronic correlations. Here we use X-ray absorption spectroscopy and resonant inelastic X-ray scattering to study the valence state of Fe and spin dynamics in two NaFe$_{1-x}$Cu$_x$As compounds ($x=0$ and 0.47). We find that magnetism in both compounds arises from Fe$^{2+}$ atoms, and exhibits underdamped dispersive spin waves in their respective ordered states. The dispersion of spin excitations in NaFe$_{0.53}$Cu$_{0.47}$As is consistent with being quasi-one-dimensional. Compared to NaFeAs, the band top of spin waves in NaFe$_{0.53}$Cu$_{0.47}$As is slightly softened with significantly more spectral weight of the spin excitations. Our results indicate the spin dynamics in NaFe$_{0.53}$Cu$_{0.47}$As arise from localized magnetic moments and suggest the iron-based superconductors are proximate to a correlated insulating state with localized iron moments.

cond-mat.str-el↗

arXiv2020

Description of resonant inelastic x-ray scattering in correlated metals

To fully capitalize on the potential and versatility of resonant inelastic x-ray scattering (RIXS), it is essential to develop the capability to interpret different RIXS contributions through calculations, including the dependence on momentum transfer, from first-principles for correlated materials. Toward that objective, we present new methodology for calculating the full RIXS response of a correlated metal in an unbiased fashion. Through comparison of measurements and calculations that tune the incident photon energy over a wide portion of the Fe L$_3$ absorption resonance of the example material BaFe$_2$As$_2$, we show that the RIXS response in BaFe$_2$As$_2$ is dominated by the direct channel contribution, including the Raman-like response below threshold, which we explain as a consequence of the finite core-hole lifetime broadening. Calculations are initially performed within the first-principles Bethe-Salpeter framework, which we then significantly improve by convolution with an effective spectral function for the intermediate-state excitation. We construct this spectral function, also from first-principles, by employing the cumulant expansion of the Green's function and performing a real-time time dependent density functional theory calculation of the response of the electronic system to the perturbation of the intermediate-state excitation. Importantly, this allows us to evaluate the indirect RIXS response from first-principles, accounting for the full periodicity of the crystal structure and with dependence on the momentum transfer.

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

Multi-orbital charge density wave excitations and concomitant phonon anomalies in Bi$_2$Sr$_2$LaCuO$_{6+δ}$

Charge density waves (CDWs) are ubiquitous in under-doped cuprate superconductors. As a modulation of the valence electron density, CDWs in hole-doped cuprates possess both Cu-3d and O-2p orbital character owing to the strong hybridization of these orbitals near the Fermi level. Here, we investigate under-doped Bi$_2$Sr$_{1.4}$La$_{0.6}$CuO$_{6+δ}$ using resonant inelastic X-ray scattering (RIXS) and find that a short-range CDW exists at both Cu and O sublattices in the copper-oxide (CuO2) planes with a comparable periodicity and correlation length. Furthermore, we uncover bond-stretching and bond-buckling phonon anomalies concomitant to the CDWs. Comparing to slightly over-doped Bi$_2$Sr$_{1.8}$La$_{0.2}$CuO$_{6+δ}$, where neither CDWs nor phonon anomalies appear, we highlight that a sharp intensity anomaly is induced in the proximity of the CDW wavevector (QCDW) for the bond-buckling phonon, in concert with the diffused intensity enhancement of the bond-stretching phonon at wavevectors much greater than QCDW. Our results provide a comprehensive picture of the quasi-static CDWs, their dispersive excitations, and associated electron-phonon anomalies, which are key for understanding the competing electronic instabilities in cuprates.

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

Reciprocity between local moments and collective magnetic excitations in the phase diagram of BaFe$_2$(As$_{1-x}$P$_x$)$_2$

Unconventional superconductivity arises at the border between the strong coupling regime with local magnetic moments and the weak coupling regime with itinerant electrons, and stems from the physics of criticality that dissects the two. Unveiling the nature of the quasiparticles close to quantum criticality is fundamental to understand the phase diagram of quantum materials. Here, using resonant inelastic x-ray scattering (RIXS) and Fe-K$_β$ emission spectroscopy (XES), we visualize the coexistence and evolution of local magnetic moments and collective spin excitations across the superconducting dome in isovalently-doped BaFe$_2$(As$_{1-x}$P$_x$)$_2$ (0.00$\leq$x$\leq0.$52). Collective magnetic excitations resolved by RIXS are gradually hardened, whereas XES reveals a strong suppression of the local magnetic moment upon doping. This relationship is captured by an intermediate coupling theory, explicitly accounting for the partially localized and itinerant nature of the electrons in Fe pnictides. Finally, our work identifies a local-itinerant spin fluctuations channel through which the local moments transfer spin excitations to the particle-hole (paramagnons) continuum across the superconducting dome.

cond-mat.supr-con↗

arXiv2019

Scale-invariant magnetic textures in the strongly correlated oxide NdNiO$_3$

Strongly correlated quantum solids are characterized by an inherently granular electronic fabric, with spatial patterns that can span multiple length scales in proximity to a critical point. Here, we used a resonant magnetic X-ray scattering nanoprobe with sub-100 nm spatial resolution to directly visualize the texture of antiferromagnetic domains in NdNiO$_3$. Surprisingly, our measurements revealed a highly textured magnetic fabric, which is shown to be robust and nonvolatile even after thermal erasure across its ordering ($T_{N\acute{e}el}$) temperature. The scale-free distribution of antiferromagnetic domains and its non-integral dimensionality point to a hitherto-unobserved magnetic fractal geometry in this system. These scale-invariant textures directly reflect the continuous nature of the magnetic transition and the proximity of this system to a critical point. The present study not only exposes the near-critical behavior in rare earth nickelates but also underscores the potential for novel X-ray scattering nanoprobes to image the multiscale signatures of criticality near a critical point.

cond-mat.str-el↗