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Gilberto Fabbris

Publications and source records attributed to Gilberto Fabbris.

At least 19 recordsLinked to original sources

Pressure tuning of competing interactions on a honeycomb lattice

Magnetic exchange interactions are mediated via orbital overlaps across chemical bonds. Thus, modifying the bond angles by physical pressure or strain can tune the relative strength of competing interactions. Here we present a remarkable case of such tuning between the Heisenberg (J) and Kitaev (K) exchange, which respectively establish magnetically ordered and spin liquid phases on a honeycomb lattice. We observe a rapid suppression of the Neel temperature (TN) with pressure in Ag3LiRh2O6, a spin-1/2 honeycomb lattice with both J and K couplings. Using a combined analysis of x-ray data and first-principles calculations, we find that pressure modifies the bond angles in a way that increases the |K/J| ratio and thereby suppresses TN. Consistent with this picture, we observe a spontaneous onset of muon spin relaxation (muSR) oscillations below TN at low pressure, whereas in the high-pressure phase, oscillations appear only when T < TN/2. Unlike other candidate Kitaev materials, Ag3LiRh2O6 is tuned toward a quantum critical point by pressure while avoiding a structural dimerization in the relevant pressure range.

cond-mat.str-el

3D Heisenberg universality in the Van der Waals antiferromagnet NiPS$_3$

Van der Waals (vdW) magnetic materials are comprised of layers of atomically thin sheets, making them ideal platforms for studying magnetism at the two-dimensional (2D) limit. These materials are at the center of a host of novel types of experiments, however, there are notably few pathways to directly probe their magnetic structure. We report the magnetic order within a single crystal of NiPS$_3$ and show it can be accessed with resonant elastic X-ray diffraction along the edge of the vdW planes in a carefully grown crystal by detecting structurally forbidden resonant magnetic X-ray scattering. We find the magnetic order parameter has a critical exponent of $\beta\sim0.36$, indicating that the magnetism of these vdW crystals is more adequately characterized by the three-dimensional (3D) Heisenberg universality class. We verify these findings with first-principle density functional theory, Monte-Carlo simulations, and density matrix renormalization group calculations.

cond-mat.str-el

Spontaneous orbital polarization in the nematic phase of FeSe

The origin of nematicity in FeSe remains a critical outstanding question towards understanding unconventional superconductivity in proximity to nematic order. To understand what drives the nematicity, it is essential to determine which electronic degree of freedom admits a spontaneous order parameter independent from the structural distortion. Here, we use X-ray linear dichroism at the Fe K pre-edge to measure the anisotropy of the 3d orbital occupation as a function of in situ applied stress and temperature across the nematic transition. Along with X-ray diffraction to precisely quantify the strain state, we reveal a lattice-independent, spontaneously-ordered orbital polarization within the nematic phase, as well as an orbital polarizability that diverges as the transition is approached from above. These results provide strong evidence that spontaneous orbital polarization serves as the primary order parameter of the nematic phase.

cond-mat.supr-con

Strain-Switchable Field-Induced Superconductivity

Field-induced superconductivity is a rare phenomenon where an applied magnetic field enhances or induces superconductivity. This fascinating effect arises from a complex interplay between magnetism and superconductivity, and it offers the tantalizing technological possibility of an infinite magnetoresistance superconducting spin valve. Here, we demonstrate field-induced superconductivity at a record-high temperature of T=9K in two samples of the ferromagnetic superconductor Eu(Fe$_{0.88}$Co$_{0.12}$)$_{2}$As$_{2}$. We combine tunable uniaxial stress and applied magnetic field to shift the temperature range of the zero-resistance state between 4K and 10K. We use x-ray diffraction and spectroscopy measurements under stress and field to demonstrate that stress tuning of the nematic order and field tuning of the ferromagnetism act as independent tuning knobs of the superconductivity. Finally, DFT calculations and analysis of the Eu dipole field reveal the electromagnetic mechanism of the field-induced superconductivity.

cond-mat.supr-con

Testing the data framework for an AI algorithm in preparation for high data rate X-ray facilities

The advent of next-generation X-ray free electron lasers will be capable of delivering X-rays at a repetition rate approaching 1 MHz continuously. This will require the development of data systems to handle experiments at these type of facilities, especially for high throughput applications, such as femtosecond X-ray crystallography and X-ray photon fluctuation spectroscopy. Here, we demonstrate a framework which captures single shot X-ray data at the LCLS and implements a machine-learning algorithm to automatically extract the contrast parameter from the collected data. We measure the time required to return the results and assess the feasibility of using this framework at high data volume. We use this experiment to determine the feasibility of solutions for `live' data analysis at the MHz repetition rate.

physics.data-an

Interplay of broken symmetry and delocalized excitations in the insulating state of 1$T$-TaS$_2$

Coexistence of localized and extended excitations is central to the macroscopic properties of correlated materials. For 5d transition metal compounds, electron correlations alone generally do not lead to a metal-insulator (Mott) transition, with insulating behavior usually resulting from their coupling with magnetic ordering and/or structural distortions. 1$T$-TaS$_2$ is a prototypical example of such correlated insulating behavior, with a high-symmetry metallic phase transforming into a distorted, charge density wave (CDW) insulating state at low temperatures. The relevance of the localized electron physics at play in 3d compounds to these 5d transition metal compounds remains an open question. We resolved this standing controversy in 1$T$-TaS$_2$ combining resonant inelastic X-ray spectroscopy and first-principles calculations. We observed five electronic excitations arising from the interband transitions of the Ta 5d orbitals and the S 3p ligand state, with none of the excitations on the order of the Mott gap. These excitations cannot be explained within the framework of standard multiplet calculations that assume a localized wavefunction, but instead, are captured by a band theory framework accounting for the low symmetry of the crystal field in the CDW state. Our findings suggest that the electronic property of 1$T$-TaS$_2$ is dominated by both plasmonic quasiparticles and inter-band transitions associated with a Drude-type response, with no resonance associated with a putative Mott transition. Our discovery provides new insights into the electron localization and the onset of insulating behavior in 5d transition metal materials.

cond-mat.mtrl-sci

Quasi-2D anomalous Hall Mott insulator of topologically engineered Jeff =1/2 electrons

We investigate an experimental toy-model system of a pseudospin-half square-lattice Hubbard Hamiltonian in [(SrIrO3)1/(CaTiO3)1] to include both nontrivial complex hopping and moderate electronic correlation. While the former induces electronic Berry phases as anticipated from the weak-coupling limit, the later stabilizes an antiferromagnetic (AFM) Mott insulator ground state in analogous to the strong-coupling limit. Their combined results in the real system are found to be an anomalous Hall effect with a non-monotonic temperature dependence due to the self-competition of the electron-hole pairing in the Mott state, and an exceptionally large Ising anisotropy that is captured as a giant magnon gap beyond the superexchange approach. The unusual phenomena highlight the rich interplay of electronic topology and electronic correlation in the intermediate-coupling regime that is largely unexplored and challenging in theoretical modelling.

cond-mat.str-el

First demonstration of tuning between the Kitaev and Ising limits in a honeycomb lattice

Recent observations of novel spin-orbit coupled states have generated tremendous interest in $4d/5d$ transition metal systems. A prime example is the $J_{\text{eff}}=\frac{1}{2}$ state in iridate materials and $\alpha$-RuCl$_{3}$ that drives Kitaev interactions. Here, by tuning the competition between spin-orbit interaction ($\lambda_{\text{SOC}}$) and trigonal crystal field splitting ($\Delta_\text{T}$), we restructure the spin-orbital wave functions into a novel $\mu=\frac{1}{2}$ state that drives Ising interactions. This is done via a topochemical reaction that converts Li$_{2}$RhO$_{3}$ to Ag$_{3}$LiRh$_{2}$O$_{6}$, leading to an enhanced trigonal distortion and a diminished spin-orbit coupling in the latter compound. Using perturbation theory, we present an explicit expression for the new $\mu=\frac{1}{2}$ state in the limit $\Delta_\text{T}\gg \lambda_{\text{SOC}}$ realized in Ag$_{3}$LiRh$_{2}$O$_{6}$, different from the conventional $J_\text{eff}=\frac{1}{2}$ state in the limit $\lambda_{\text{SOC}}\gg \Delta_\text{T}$ realized in Li$_{2}$RhO$_{3}$. The change of ground state is followed by a dramatic change of magnetism from a 6 K spin-glass in Li$_{2}$RhO$_{3}$ to a 94 K antiferromagnet in Ag$_{3}$LiRh$_{2}$O$_{6}$. These results open a pathway for tuning materials between the two limits and creating a rich magnetic phase diagram.

cond-mat.mtrl-sci

Pressure-induced charge orders and their coupling to magnetism in hexagonal multiferroic LuFe2O4

Hexagonal LuFe2O4 is a promising charge-order (CO) driven multiferroic material with high charge and spin ordering temperatures. The coexisting charge and spin orders on Fe3+/Fe2+ sites result in novel magnetoelectric behaviors, but the coupling mechanism between the charge and spin orders remains elusive. Here, by tuning external pressure, we reveal three correlated spin-charge ordered phases in LuFe2O4: i) a centrosymmetric incommensurate three-dimensional CO with ferrimagnetism, ii) a non-centrosymmetric incommensurate quasi-two-dimensional CO with ferrimagnetism, and iii) a centrosymmetric commensurate CO with antiferromagnetism. Experimental in-situ single-crystal X-ray diffraction and X-ray magnetic circular dichroism measurements combined with density functional theory calculations suggest that the charge density redistribution caused by pressure-induced compression in the frustrated double-layer [Fe2O4] cluster is responsible for the correlated spin-charge phase transitions. The pressure-enhanced effective Coulomb interactions among Fe-Fe bonds drive the frustrated (1/3, 1/3) CO to a less frustrated (1/4, 1/4) CO, which induces the ferrimagnetic to antiferromagnetic transition. Our results not only elucidate the coupling mechanism among charge, spin and lattice degrees of freedom in LuFe2O4 but also provide a new way to tune the spin-charge orders in a highly controlled manner.

cond-mat.mtrl-sci

A magnetic Weyl semimetallic phase in thin films of Eu$_2$Ir$_2$O$_7$

The interplay between electronic interactions and strong spin-orbit coupling is expected to create a plethora of fascinating correlated topological states of quantum matter. Of particular interest are magnetic Weyl semimetals originally proposed in the pyrochlore iridates, which are only expected to reveal their topological nature in thin film form. To date, however, direct experimental demonstrations of these exotic phases remain elusive, due to the lack of usable single crystals and the insufficient quality of available films. Here, we report on the discovery of the long-sought magnetic Weyl semi-metallic phase in (111)-oriented Eu$_2$Ir$_2$O$_7$ high-quality epitaxial thin films. The topological magnetic state shows an intrinsic anomalous Hall effect with colossal coercivity but vanishing net magnetization, which emerges below the onset of a peculiar magnetic phase with all-in-all-out antiferromagnetic ordering. The observed anomalous Hall conductivity arises from the non-zero Berry curvature emanated by Weyl node pairs near the Fermi level that act as sources and sinks of Berry flux, activated by broken cubic crystal symmetry at the top and bottom terminations of the thin film.

cond-mat.str-el

Giant anisotropic magnetoresistance with dual-four-fold symmetry in CaMnO3/CaIrO3 heterostructures

The realization of four-fold anisotropic magnetoresistance (AMR) in novel 3d-5d heterostructures has boosted major efforts in antiferromagnetic spintronics. However, despite the potential of incorporating strong spin-orbit coupling, only small AMR signals have been detected thus far, prompting a search for new mechanisms to enhance the signal. In this study on CaMnO3/CaIrO3 heterostructures, we report a unique dual-four-fold symmetric 70% AMR; a signal two orders of magnitude larger than previously observed in similar systems. We find that one order is enhanced by tuning a large biaxial anisotropy through octahedral tilts of similar sense in the constituent layers, while the second order is triggered by a spin-flop transition in a nearly Mott-type phase. Dynamics between these two phenomena as evidenced by the step-like AMR and a superimposed biaxial-anisotropy-induced AMR capture a subtle interplay of pseudospin coupling with the lattice and external magnetic field. Our study shows that a combination of charge-transfer, interlayer coupling, and a spin-flop transition can yield a giant AMR relevant for sensing and antiferromagnetic memory applications.

cond-mat.mtrl-sci

Strongly anisotropic antiferromagnetic coupling in EuFe2As2 revealed by stress detwinning

Of all parent compounds of iron-based high-temperature superconductors, EuFe2As2 exhibits by far the largest magnetostructural coupling due to the sizable biquadratic interaction between Eu and Fe moments. While the coupling between Eu antiferromagnetic order and Fe structural/antiferromagnetic domains enables rapid field detwinning, this prevents simple magnetometry measurements from extracting the critical fields of the Eu metamagnetic transition. Here we measure these critical fields by combining x-ray magnetic circular dichroism spectroscopy with in-situ tunable uniaxial stress and applied magnetic field. The combination of two tuning knobs allows us to separate the stress-detwinning of structural domains from the field-induced reorientation of Eu moments. Intriguingly, we find a spin-flip transition which can only result from a strongly anisotropic interaction between Eu planes. We argue that this anisotropic exchange is a consequence of the strong anisotropy in the magnetically ordered Fe layer, which presents a new form of higher-order coupling between Eu and Fe magnetism.

cond-mat.supr-con

Strain-modulated Slater-Mott crossover of pseudospin-half square-lattice in (SrIrO3)1/ (SrTiO3)1 superlattices

We report on the epitaxial strain-driven electronic and antiferromagnetic modulations of a pseudospin-half square lattice realized in superlattices of (SrIrO3)1/(SrTiO3)1. With increasing compressive strain, we find the low-temperature insulating behavior to be strongly suppressed with a corresponding systematic reduction of both the Neel temperature and the staggered moment. However, despite such a suppression, the system remains weakly insulating above the Neel transition. The emergence of metallicity is observed under large compressive strain but only at temperatures far above the Néel transition. These behaviors are characteristics of the Slater-Mott crossover regime, providing a unique experimental model system of the spin-half Hubbard Hamiltonian with a tunable intermediate coupling strength.

cond-mat.str-el

Machine learning spectral indicators of topology

Topological materials discovery has emerged as an important frontier in condensed matter physics. While theoretical classification frameworks have been used to identify thousands of candidate topological materials, experimental determination of materials' topology often poses significant technical challenges. X-ray absorption spectroscopy (XAS) is a widely-used materials characterization technique sensitive to atoms' local symmetry and chemical bonding, which are intimately linked to band topology by the theory of topological quantum chemistry (TQC). Moreover, as a local structural probe, XAS is known to have high quantitative agreement between experiment and calculation, suggesting that insights from computational spectra can effectively inform experiments. In this work, we leverage computed X-ray absorption near-edge structure (XANES) spectra of more than 10,000 inorganic materials to train a neural network (NN) classifier that predicts topological class directly from XANES signatures, achieving F$_1$ scores of 89% and 93% for topological and trivial classes, respectively. Additionally, we obtain consistent classifications using corresponding experimental and computational XANES spectra for a small number of measured compounds. Given the simplicity of the XAS setup and its compatibility with multimodal sample environments, the proposed machine learning-augmented XAS topological indicator has the potential to discover broader categories of topological materials, such as non-cleavable compounds and amorphous materials, and may further inform field-driven phenomena in situ, such as magnetic field-driven topological phase transitions.

cond-mat.dis-nn

Anomalous Magnetoresistance due to Longitudinal Spin Fluctuations in a Jeff = 1/2 Mott Semiconductor

As a hallmark of electronic correlation, spin-charge interplay underlies many emergent phenomena in doped Mott insulators, such as high-temperature superconductivity, whereas the half-filled parent state is usually electronically frozen with an antiferromagnetic order that resists external control. We report on the observation of a new positive magnetoresistance that probes the staggered susceptibility of a pseudospin-half square-lattice Mott insulator built as an artificial SrIrO3/SrTiO3 superlattice. Its size is particularly large in the high-temperature insulating paramagnetic phase near the Néel transition. This novel magnetoresistance originates from a collective charge response to the large longitudinal spin fluctuations under a linear coupling between the external magnetic field and the staggered magnetization enabled by strong spin-orbit interaction. Our results demonstrate a magnetic control of the binding energy of the fluctuating particle-hole pairs in the Slater-Mott crossover regime analogous to the BCS-to-Bose-Einstein condensation crossover of ultracold-superfluids.

cond-mat.str-el

Inverted orbital polarization in strained correlated oxide films

Manipulating the orbital occupation of valence electrons via epitaxial strain in an effort to induce new functional properties requires considerations of how changes in the local bonding environment affect the band structure at the Fermi level. Using synchrotron radiation to measure the x-ray linear dichroism of epitaxially strained films of the correlated oxide CaFeO3, we demonstrate that the orbital polarization of the Fe valence electrons is opposite from conventional understanding. Although the energetic ordering of the Fe 3d orbitals is confirmed by multiplet ligand field theory analysis to be consistent with previously reported strain-induced behavior, we find that the nominally higher energy orbital is more populated than the lower. We ascribe this inverted orbital polarization to an anisotropic bandwidth response to strain in a compound with nearly filled bands. These findings provide an important counterexample to the traditional understanding of strain-induced orbital polarization and reveal a new method to engineer otherwise unachievable orbital occupations in correlated oxides.

cond-mat.str-el

Competition between static and dynamic magnetism in the Kitaev spin liquid material Cu2IrO3

Anyonic excitations emerging from a Kitaev spin liquid can form a basis for quantum computers. Searching for such excitations motivated intense research on the honeycomb iridate materials. However, access to a spin liquid ground state has been hindered by magnetic ordering. Cu2IrO3 is a new honeycomb iridate without thermodynamic signatures of a long-range order. Here, we use muon spin relaxation to uncover the magnetic ground state of Cu2IrO3. We find a two-component depolarization with slow and fast relaxation rates corresponding to distinct regions with dynamic and static magnetism, respectively. X-ray absorption spectroscopy and first principles calculations identify a mixed copper valence as the origin of this behavior. Our results suggest that a minority of Cu2+ ions nucleate regions of static magnetism whereas the majority of Cu+/Ir4+ on the honeycomb lattice give rise to a Kitaev spin liquid.

cond-mat.str-el

Giant magnetic response of a two-dimensional antiferromagnet

A fundamental difference between antiferromagnets and ferromagnets is the lack of linear coupling to a uniform magnetic field due to the staggered order parameter. Such coupling is possible via the Dzyaloshinskii-Moriya (DM) interaction but at the expense of reduced antiferromagnetic (AFM) susceptibility due to the canting-induced spin anisotropy. We solve this long-standing problem with a top-down approach that utilizes spin-orbit coupling in the presence of a hidden SU(2) symmetry. We demonstrate giant AFM responses to sub-Tesla external fields by exploiting the extremely strong two-dimensional critical fluctuations preserved under a symmetry-invariant exchange anisotropy, which is built into a square-lattice artificially synthesized as a superlattice of SrIrO3 and SrTiO3. The observed field-induced logarithmic increase of the ordering temperature enables highly efficient control of the AFM order. As antiferromagnets promise to afford switching speed and storage security far beyond ferromagnets, our symmetry-invariant approach unleashes the great potential of functional antiferromagnets.

cond-mat.str-el