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G. Fabbris

Publications and source records attributed to G. Fabbris.

At least 19 recordsLinked to original sources

Revealing magnetism in the distorted kagome $R$Ti$_3$Bi$_4$ ($R$ = Nd, Sm, Gd) via ARPES and XMCD

Kagome materials are known for hosting emergent quantum phenomena driven by the interaction between different lattice, charge and spin orders. Here, we present a detailed angle resolved photoemission (ARPES), density functional theory (DFT) and x-ray magnetic circular dichroism (XMCD) study of the electronic and magnetic structure of $R$Ti$_3$Bi$_4$ ($R$ = Nd, Sm, Gd). ARPES and DFT demonstrate that the bulk electronic band structure is dominated by the hybridization of the Ti bands, and the weak electron-like pocket at $\Gamma$ is identified as a surface state. The isotropic XAS profile of the $M_{4,5}$-edge of the rare earth is consistent with the presence of $R^{3+}$ oxidation state. Using the XMCD sum rules, backed by the atomic multiplet theory calculations, we obtain the spin and orbital magnetic moments. The Ti $L_{2,3}$-edge XMCD reveals the presence of a small magnetic moment in GdTi$_3$Bi$_4$, presumably driven by the proximity of the {Ti} kagome layers to the $zigzag$ chains of Gd, while the total magnetic moment of Gd is shared by the $f$ and $d$ electrons. Our combined XMCD, ARPES and DFT study brings an important piece of information to understand the spin flip transitions and anomalous Hall effect observed in the $R$Ti$_3$Bi$_4$ kagome metals.

cond-mat.mtrl-sci

Magnetic Imaging of Macroscopic Spin Chirality Flipping

Chirality is a fundamental organizing principle of correlated and topological states. In quantum magnets, chirality arises from the geometric twisting of spins and serves as an emergent source of Berry curvature and quantum metrics. Although external fields can reversibly tune the spin chirality, understanding how spontaneous reversal occurs on macroscopic length scale remains an unresolved challenge. In this letter, we use resonant magnetic x-ray scattering with 2.5-micron spatial resolution to image intertwined spin, charge, and lattice orders of the correlated topological magnet EuAl4. We uncover a macroscopic chirality flipping transition and a remarkable chiral memory effect. The chiral magnetic domain tracks the landscape of the underlying charge density wave, implicating emergent chiral magnetic interactions arising from competing chiral and nematic lattice fields. Our results reveal the fundamental significance of magnetoelastic coupling in stabilizing homochiral and topological magnetic states.

cond-mat.str-el

Pressure tuning of Kitaev spin liquid candidate Na$_3$Co$_2$SbO$_6$

The search for Kitaev's quantum spin liquid (KQSL) state in real materials has recently expanded with the prediction that honeycomb lattices of divalent, high-spin cobalt ions could host the dominant bond-dependent exchange interactions required to stabilize the elusive entangled quantum state. The layered honeycomb Na$_3$Co$_2$SbO$_6$ has been singled out as a leading candidate provided that the trigonal crystal field acting on Co $3d$ orbitals, which enhances non-Kitaev exchange interactions between $J_{\rm eff}=\frac{1}{2}$ spin-orbital pseudospins, is reduced. We find that applied pressure leads to anisotropic compression of the layered structure, significantly reducing the trigonal distortion of CoO$_6$ octahedra. A strong enhancement of ferromagnetic correlations between pseudospins is observed in the spin-polarized (3 Tesla) phase up to about 60 GPa. Higher pressures drive a spin transition into a low-spin state destroying the $J_{\rm eff}=\frac{1}{2}$ local moments required to map the spin Hamiltonian into Kitaev's model. The spin transition strongly suppresses the low-temperature magnetic susceptibility and appears to stabilize a paramagnetic phase driven by frustration. Although applied pressure fails to realize a KQSL state, the possible emergence of frustrated magnetism of localized, low-spin $S=\frac{1}{2}$ moments opens the door for exploration of novel magnetic quantum states in compressed honeycomb lattices of divalent cobaltates.

cond-mat.str-el

Incommensurate Transverse Peierls Transition

In one-dimensional quantum materials, conducting electrons and the underlying lattices can undergo a spontaneous translational symmetry breaking, known as Peierls transition. For nearly a century, the Peierls transition has been understood within the paradigm of electron-electron interactions mediated by longitudinal acoustic phonons. This classical picture has recently been revised in topological semimetals, where transverse acoustic phonons can couple with conducting p-orbital electrons and give rise to an unconventional Fermi surface instability, dubbed the transverse Peierls transition (TPT). Most interestingly, the TPT induced lattice distortions can further break rotation or mirror/inversion symmetries, leading to nematic or chiral charge density waves (CDWs). Quantum materials that host the TPT, however, have not been experimentally established. Here, we report the experimental discovery of an incommensurate TPT in the tetragonal Dirac semimetal EuAl$_4$. Using inelastic x-ray scattering with meV resolution, we observe the complete softening of a transverse acoustic phonon at the CDW wavevector upon cooling, whereas the longitudinal acoustic phonon is nearly unchanged. Combining with first principles calculations, we show that the incommensurate CDW wavevector matches the calculated charge susceptibility peak and connects the nested Dirac bands with Al 3$p_{x}$ and 3$p_{y}$ orbitals. Supplemented by second harmonic generation measurements, we show that the CDW induced lattice distortions break all vertical and diagonal mirrors whereas the four-fold rotational symmetry is retained below the CDW transition. Our observations strongly suggest a chiral CDW in EuAl$_4$ and highlight the TPT as a new avenue for chiral quantum states.

cond-mat.str-el

Novel electronic state of honeycomb iridate Cu$_2$IrO$_3$ at high pressure

Cu$_2$IrO$_3$ has attracted recent interest due to its proximity to the Kitaev quantum spin liquid state and the complex structural response observed at high pressures. We use x-ray spectroscopy and scattering as well as electrical transport techniques to unveil the electronic structure of Cu$_2$IrO$_3$ at ambient and high pressures. Despite featuring a $\mathrm{Ir^{4+}}$ $J_{\rm{eff}}=1/2$ state at ambient pressure, Ir $L_{3}$ edge resonant inelastic x-ray scattering reveals broadened electronic excitations that point to the importance of Ir $5d$-Cu $3d$ interaction. High pressure first drives an Ir-Ir dimer state with collapsed $\langle \mathbf{L} \cdot \mathbf{S} \rangle$ and $\langle L_z \rangle/\langle S_z \rangle$, signaling the formation of $5d$ molecular orbitals. A novel $\mathrm{Cu \to Ir}$ charge transfer is observed at the onset of phase 5 above 30 GPa at low temperatures, leading to an approximate $\mathrm{Ir^{3+}}$ and $\mathrm{Cu^{1.5+}}$ valence, with persistent insulating electrical transport seemingly driven by charge segregation of Cu 1+/2+ ions into distinct sites. Concomitant x-ray spectroscopy and scattering measurements through different thermodynamic paths demonstrate a strong electron-lattice coupling, with $J_{\rm{eff}}=1/2$ and $\mathrm{Ir^{3+}}$/$\mathrm{Cu^{1.5+}}$ electronic states occurring only in phases 1 and 5, respectively. Remarkably, the charge-transferred state can only be reached if Cu$_2$IrO$_3$ is pressurized at low temperature, suggesting that phonons play an important role in the stability of this phase. These results point to the choice of thermodynamic path across interplanar collapse transition as a key route to access novel states in intercalated iridates.

cond-mat.str-el

Charge Density Waves in the 2.5-Dimensional Quantum Heterostructure

Charge density wave (CDW) and their interplay with correlated and topological quantum states are forefront of condensed matter research. The 4$H_{b}$-TaS$_2$ is a CDW ordered quantum heterostructure that is formed by alternative stacking of Mott insulating 1T-TaS$_2$ and Ising superconducting 1H-TaS$_2$. While the $\sqrt{13}\times\sqrt{13}$ and 3$\times$3 CDWs have been respectively observed in the bulk 1T-TaS$_2$ and 2H-TaS$_2$, the CDWs and their pivotal role for unconventional superconductivity in the 4$H_{b}$-TaS$_2$ remain unsolved. In this letter, we reveal the 2-dimensional (2D) $\sqrt{13}\times\sqrt{13}$ chiral CDW in the 1T-layers and intra-unit cell coupled 2D 2$\times$2 CDW in the 1H and 1H' layers of 4$H_{b}$-TaS$_2$. Our results establish 4$H_{b}$-TaS$_2$ a novel 2.5D quantum heterostructure, where 2D quantum states emerge from 3D crystalline structure.

cond-mat.supr-con

Signature of Orbital Driven Finite Momentum Pairing in a 3D Ising Superconductor

The finite momentum superconducting pairing states (FMPs), where Cooper pairs carry non-zero momentum, are believed to give rise to exotic physical phenomena including the pseudogap phase of cuprate high-Tc superconductors and Majorana fermions in topological superconductivity. FMPs can emerge in intertwined electronic liquids with strong spin-spin interactions or be induced by lifting the spin degeneracy under magnetic field as originally proposed by Fulde-Ferrell and Larkin-Ovchinnikov. In quantum materials with strong Ising-type spin-orbit coupling, such as the 2D transition metal dichalcogenides (TMDs), the spin degree of freedom is frozen enabling novel orbital driven FMPs via magnetoelectric effect. While evidence of orbital driven FMPs has been revealed in bilayer TMDs, its realization in 3D bulk materials remains an unresolved challenge. Here we report experimental signatures of FMP in a locally noncentrosymmetric bulk superconductor 4Hb-TaS2. Using hard X-ray diffraction and angle-resolved photoemission spectroscopy, we reveal unusual 2D chiral charge density wave (CDW) and weak interlayer hopping in 4Hb-TaS2. Below the superconducting transition temperature, the upper critical field, Hc2, linearly increases via decreasing temperature, and well exceeds the Pauli limit, thus establishing the dominant orbital pair-breaking mechanism. Remarkably, we discover a field-induced superconductivity-to-superconductivity transition that breaks continuous rotational symmetry of the s-wave uniform pairing in the Bardeen-Cooper-Schrieffer theory down to the six-fold rotation symmetry. Combining with a Ginzburg-Landau free energy analysis that incorporates magnetoelectric effect, our observations provide strong evidence of orbital driven FMP in the 3D quantum heterostructure 4Hb-TaS2.

cond-mat.supr-con

Spontaneous Chirality Flipping in an Orthogonal Spin-Charge Ordered Topological Magnet

The asymmetric distribution of chiral objects with opposite chirality is of great fundamental interests ranging from molecular biology to particle physics. In quantum materials, chiral states can build on inversion-symmetry-breaking lattice structures or emerge from spontaneous magnetic ordering induced by competing interactions. Although the handedness of a chiral state can be changed through external fields, a spontaneous chirality flipping has yet to be discovered. In this letter, we present experimental evidence of chirality flipping via changing temperature in a topological magnet EuAl$_4$, which features orthogonal spin and charge density waves (SDW/CDW). Using circular dichroism of Bragg peaks in the resonant magnetic x-ray scattering, we find that the chirality of the helical SDW flips through a first order phase transition with modified SDW wavelength. Intriguingly, we observe that the CDW couples strongly with the SDW and displays a rare commensurate-to-incommensurate transition at the chirality flipping temperature. Combining with first principles calculations and angle resolved photoemission spectroscopy, we establish the Fermi surface origin of the helical SDW with intertwined spin, charge, and lattice degrees of freedom in EuAl$_4$. Our results reveal an unprecedented spontaneous chirality flipping and lays the groundwork for a new functional manipulation of chirality through momentum dependent spin-charge-lattice interactions.

cond-mat.str-el

Quantum spin nematic phase in a square-lattice iridate

Spin nematic (SN) is a magnetic analog of classical liquid crystals, a fourth state of matter exhibiting characteristics of both liquid and solid. Particularly intriguing is a valence-bond SN, in which spins are quantum entangled to form a multi-polar order without breaking time-reversal symmetry, but its unambiguous experimental realization remains elusive. Here, we establish a SN phase in the square-lattice iridate Sr$_2$IrO$_4$, which approximately realizes a pseudospin one-half Heisenberg antiferromagnet (AF) in the strong spin-orbit coupling limit. Upon cooling, the transition into the SN phase at T$_C$ $\approx$ 263 K is marked by a divergence in the static spin quadrupole susceptibility extracted from our Raman spectra, and concomitant emergence of a collective mode associated with the spontaneous breaking of rotational symmetries. The quadrupolar order persists in the antiferromagnetic (AF) phase below T$_N$ $\approx$ 230 K, and becomes directly observable through its interference with the AF order in resonant x-ray diffraction, which allows us to uniquely determine its spatial structure. Further, we find using resonant inelastic x-ray scattering a complete breakdown of coherent magnon excitations at short-wavelength scales, suggesting a resonating-valence-bond-like quantum entanglement in the AF state. Taken together, our results reveal a quantum order underlying the Néel AF that is widely believed to be intimately connected to the mechanism of high temperature superconductivity (HTSC).

cond-mat.str-el

Helical magnetic state in the vicinity of the pressure-induced superconducting phase in MnP

MnP is a metal that shows successive magnetic transitions from paramagnetic to ferromagnetic and helical magnetic phases at ambient pressure with decreasing temperature. With applied pressure, the magnetic transition temperatures decrease and superconductivity appears around 8 GPa where the magnetic order is fully suppressed and the quantum critical behavior is observed. These results suggest that MnP is an unconventional superconductor in which magnetic fluctuations may be relevant to the superconducting pairing mechanism. In order to elucidate the magnetic ground state adjacent to the superconducting phase first discovered in Mn-based materials, high-pressure neutron diffraction measurements have been performed in hydrostatic pressure up to 7.5 GPa. The helical magnetic structure with the propagation vector along the $b$ axis, reported previously at 3.8 GPa, was found to be robust up to 7.5 GPa. First principles and classical Monte Carlo calculations have also been performed to understand how the pressure-driven magnetic phase transitions are coupled with change of the exchange interactions. The calculations, which qualitatively reproduce the magnetic structures as a function of pressure, suggest that the exchange interactions change drastically with applied pressure and the further-neighbor interactions become more influential at high pressures. Combining the experimental and theoretical results, we describe the detail of exchange interactions in the vicinity of the superconducting phase which is critical to understand the pairing mechanism of the unconventional superconductivity in MnP.

cond-mat.mtrl-sci

Orbital polarization, charge transfer, and fluorescence in reduced valence nickelates

This paper presents a simple formalism for calculating X-ray absorption (XAS) and resonant inelastic x-ray scattering (RIXS) that has as input orbital-resolved density of states from a single-particle or many-body \textit{ab initio} calculation and is designed to capture itinerant-like features. We use this formalism to calculate both the XAS and RIXS with input from DFT and DFT+DMFT for the recently studied reduced valence nickelates $R_4$Ni$_3$O$_8$ and $R$NiO$_2$ ($R$ a rare earth), and these results are then contrasted with those for the cuprate CaCuO$_2$ and the unreduced nickelate $R_4$Ni$_3$O$_{10}$. In contrast to the unreduced $R_4$Ni$_3$O$_{10}$, the reduced valence nickelates as well as the cuprate show strong orbital polarization due to the dominance of $x^2-y^2$ orbitals for the unoccupied $3d$ states. We also reproduce two key aspects of a recent RIXS experiment for $R_4$Ni$_3$O$_8$: (i) a charge transfer feature between $3d$ and oxygen $2p$ states whose energy we find to decrease as one goes from $R$NiO$_2$ to $R_4$Ni$_3$O$_8$ to the cuprate, and (ii) an energy-dependent polarization reversal of the fluorescence line that arises from hybridization of the unoccupied $z^2$ states with $R$ 5d states. We end with some implications of our results for the nature of the $3d$ electrons in reduced valence nickelates.

cond-mat.str-el

Resonant inelastic x-ray scattering data for Ruddlesden-Popper and reduced Ruddlesden-Popper nickelates

Ruddlesden-Popper and reduced Ruddlesden-Popper nickelates are intriguing candidates for mimicking the properties of high-temperature superconducting cuprates. The degree of similarity between these nickelates and cuprates has been the subject of considerable debate. Resonant inelastic x-ray scattering (RIXS) has played an important role in exploring their electronic and magnetic excitations, but these efforts have been stymied by inconsistencies between different samples and the lack of publicly available data for detailed comparison. To address this issue, we present open RIXS data on La4Ni3O10 and La4Ni3O8.

cond-mat.str-el

Momentum-independent magnetic excitation continuum in the honeycomb iridate H$_3$LiIr$_2$O$_6$

In the search for realizations of Quantum Spin Liquids (QSL), it is essential to understand the interplay between inherent disorder and the correlated fluctuating spin ground state. H$_3$LiIr$_2$O$_6$ is regarded as a spin liquid proximate to the Kitaev-limit (KQSL) in which H zero-point motion and stacking faults are known to be present. Bond disorder has been invoked to account for the existence of unexpected low-energy spin excitations. Controversy remains about the nature of the underlying correlated state and if any KQSL physics survives. Here, we use resonant X-ray spectroscopies to map the collective excitations in H$_3$LiIr$_2$O$_6$ and characterize its magnetic state. We uncover a broad bandwidth and momentum-independent continuum of magnetic excitations at low temperatures that are distinct from the paramagnetic state. The center energy and high-energy tail of the continuum are consistent with expectations for dominant ferromagnetic Kitaev interactions between dynamically fluctuating spins. The absence of a momentum dependence to these excitations indicates a broken translational invariance. Our data support an interpretation of H$_3$LiIr$_2$O$_6$ as a disordered topological spin liquid in close proximity to bond-disordered versions of the KQSL. Our results shed light on how random disorder affects topological magnetic states and have implications for future experimental and theoretical works toward realizing the Kitaev model in condensed matter systems

cond-mat.str-el

Electronic character of charge order in square planar low valence nickelates

Charge order is a central feature of the physics of cuprate superconductors and is known to arise from a modulation of holes with primarily oxygen character. Low-valence nickelate superconductors also host charge order, but the electronic character of this symmetry breaking is unsettled. Here, using resonant inelastic x-ray scattering at the Ni $L_2$-edge, we identify intertwined involvements of Ni $3d_{x^2-y^2}$, $3d_{3z^2-r^2}$, and O $2p_σ$ orbitals in the formation of diagonal charge order in an overdoped low-valence nickelate La$_{4}$Ni$_{3}$O$_{8}$. The Ni $3d_{x^2-y^2}$ orbitals, strongly hybridized with planar O $2p_σ$, largely shape the spatial charge distribution and lead to Ni site-centered charge order. The $3d_{3z^2-r^2}$ orbitals play a small, but non-negligible role in the charge order as they hybridize with the rare-earth $5d$ orbitals. Our results reveal that the low-energy physics and ground-state character of these nickelates are more complex than those in cuprates.

cond-mat.str-el

Spin-phonon coupling driven Charge density wave in a Kagome Magnet

The intertwining between spin, charge, and lattice degrees of freedom can give rise to unusual macroscopic quantum states, including high-temperature superconductivity and quantum anomalous Hall effects. Recently, a charge density wave (CDW) is observed in the kagome antiferromagnet FeGe, indicative of possible intertwining physics. An outstanding question is that whether magnetic correlation is fundamental for the spontaneous spatial symmetry breaking orders. Here, utilizing elastic and high-resolution inelastic x-ray scattering, we discover a charge dimerization superlattice that coexists with the 2$\times$2$\times$1 CDW in the kagome sublattice. Most interestingly, between the magnetic and CDW transition temperature, the phonon dynamical structure factor shows a giant phonon-energy hardening and a substantial phonon linewidth broadening near the charge-dimerization wavevectors, both signaling the spin-phonon coupling. By first principles calculations, we show that both the static and dynamic spin excitations intertwine with the phonon to drive the spatial symmetry breaking.

cond-mat.str-el

Emergence of spinons in layered trimer iridate Ba4Ir3O10

Spinons are well-known as the elementary excitations of one-dimensional antiferromagnetic chains, but means to realize spinons in higher dimensions is the subject of intense research. Here, we use resonant x-ray scattering to study the layered trimer iridate Ba4Ir3O10, which shows no magnetic order down to 0.2 K. An emergent one-dimensional spinon continuum is observed that can be well-described by XXZ spin-1/2 chains with magnetic exchange of ~55 meV and a small Ising-like anisotropy. With 2% isovalent Sr doping, magnetic order appears below TN=130 K along with sharper excitations, indicating that the spinons become more confined in (Ba1-xSrx)4Ir3O10. We propose that the frustrated intra-trimer interactions effectively reduce the system into decoupled spin chains, the subtle balance of which can be easily tipped by perturbations such as chemical doping. Our results put Ba4Ir3O10 between the one-dimensional chain and two-dimensional quantum spin liquid scenarios, illustrating a new way to suppress magnetic order and realize fractional spinons.

cond-mat.str-el

Nanometric modulations of the magnetic structure of the element Nd

The rare earth neodymium arguably exhibits the most complex magnetic ordering and series of magnetic phase transitions of the elements. Here we report the results of small-angle neutron scattering (SANS) measurements as a function of temperature and applied magnetic field to study magnetic correlations on nanometer length scales in Nd. The SANS measurements reveal the presence of previously unreported modulation vectors characterizing the ordered spin configuration which exhibit changes in magnitude and direction that are phase dependent. Between 5.9 and 7.6 K the additional modulation vector has a magnitude $Q$ =0.12 Å$^{-1}$ and is primarily due to order of the Nd layers which contain a center of inversion. In this region of the phase diagram, the SANS measurements also identify a phase boundary at $\approx$1 T. An important feature of these modulation vectors is that they indicate the presence of nanometer length scale spin textures which are likely stabilized by frustrated Ruderman-Kittel-Kasuya-Yosida (RKKY) interactions rather than a Dzyaloshinskii-Moriya (DM) exchange interaction.

cond-mat.str-el

On the electronic ground state of two non-magnetic pentavalent honeycomb iridates

We investigate the electronic structure of two Ir$^{5+}$ honeycomb iridates, Sr$_3$CaIr$_2$O$_9$ and NaIrO$_3$, by means of resonant x-ray techniques. We confirm that Sr$_3$CaIr$_2$O$_9$ realizes a large spin-orbit driven non-magnetic $J = 0$ singlet ground state despite sizable tetragonal distortions of Ir coordinating octahedra. On the other hand, the resonant inelastic x-ray spectra of NaIrO$_3$ are drastically different from expectations for a Mott insulator with octahedrally coordinated Ir$^{5+}$. We find that the data for NaIrO$_3$ can be best interpreted as originating from a narrow gap non-magnetic $S = 0$ band insulating ground state. Our results highlight the complex role of the ligand environment in the electronic structure of honeycomb iridates and the essential role of x-ray spectroscopy to characterize electronic ground states of insulating materials.

cond-mat.str-el