arXiv subjects

Alex Frano

Publications and source records attributed to Alex Frano.

At least 37 records · Page 2Linked to original sources

arXiv2022

Antiferromagnetic order in Co-doped Fe$_5$GeTe$_2$ probed by resonant magnetic x-ray scattering

The quasi-two-dimensional van der Waals magnet Fe$_{5-δ}$GeTe$_2$ has emerged as a promising platform for electronic and spintronic functionalities at room temperature, owing to its large ferromagnetic ordering temperature $T_{\text{C}}$ $\sim$ 315 K. Interestingly, by cobalt (Co) substitution of iron in F5GT, $i.e.$ $({\text{Fe}}_{1-x}{\text{Co}}_x)_{5-δ}{\text{GeTe}}_2$ (Co-F5GT), not only can its magnetic transition temperature be further enhanced, but the magnetic and structural ground states can also be tuned. Specifically, an antiferromagnetic (AFM) order is induced beyond the Co doping level $x \ge 0.4$. Here, we investigate the magnetic properties of a Co-F5GT single crystal at $x = 0.45(1)$, by utilizing the element specific, resonant magnetic x-ray scattering technique. Our study reveals an A-type, Ising-like AFM ground state, with a transition temperature $T_{\text{N}}$ $\sim$ 340 K. In addition, our work unveils an important contribution from Co magnetic moments to the magnetic order. The application of the in-plane magnetic fields gradually polarize the spin moments along the field direction, but without inducing incommensurate spin texture(s).

cond-mat.mtrl-sci↗

arXiv2022

Quantum materials for energy-efficient neuromorphic computing

Neuromorphic computing approaches become increasingly important as we address future needs for efficiently processing massive amounts of data. The unique attributes of quantum materials can help address these needs by enabling new energy-efficient device concepts that implement neuromorphic ideas at the hardware level. In particular, strong correlations give rise to highly non-linear responses, such as conductive phase transitions that can be harnessed for short and long-term plasticity. Similarly, magnetization dynamics are strongly non-linear and can be utilized for data classification. This paper discusses select examples of these approaches, and provides a perspective for the current opportunities and challenges for assembling quantum-material-based devices for neuromorphic functionalities into larger emergent complex network systems.

cs.ET↗

arXiv2022

Stabilization of three-dimensional charge order through interplanar orbital hybridization in Pr$_x$Y$_{1-x}$Ba$_2$Cu$_3$O$_{6+δ}$

The shape of 3$d$-orbitals often governs the electronic and magnetic properties of correlated transition metal oxides. In the superconducting cuprates, the planar confinement of the $d_{x^2-y^2}$ orbital dictates the two-dimensional nature of the unconventional superconductivity and a competing charge order. Achieving orbital-specific control of the electronic structure to allow coupling pathways across adjacent planes would enable direct assessment of the role of dimensionality in the intertwined orders. Using Cu-$L_3$ and Pr-$M_5$ resonant x-ray scattering and first-principles calculations, we report a highly correlated three-dimensional charge order in Pr-substituted YBa$_2$Cu$_3$O$_{7}$, where the Pr $f$-electrons create a direct orbital bridge between CuO$_2$ planes. With this, we demonstrate that interplanar orbital engineering can be used to surgically control electronic phases in correlated oxides and other layered materials.

cond-mat.str-el↗

arXiv2021

Low-temperature emergent neuromorphic networks with correlated oxide devices

Neuromorphic computing which aims to mimic the collective and emergent behavior of the brain's neurons, synapses, axons, dendrites offers an intriguing, potentially disruptive solution to society's ever-growing computational needs. Although much progress has been made in designing circuit elements that mimic the behavior of neurons and synapses, challenges remain in designing networks of elements that feature a collective response behavior. We present simulations of networks of circuits and devices based on superconducting and Mott-insulating oxides that display a multiplicity of emergent states that depend on the spatial configuration of the network. Our proposed network designs are based on experimentally known ways of tuning the properties of these oxides using light ions. We show how neuronal and synaptic behavior can be achieved with arrays of superconducting Josephson junction loops, all within the same device. We also show how a multiplicity of synaptic states could be achieved by designing arrays of devices based on hydrogenated rare-earth nickelates. Together, our results demonstrate a new research platform that utilizes the collective macroscopic properties of quantum materials to mimic the emergent behavior found in biological systems.

physics.app-ph↗

arXiv2021

Proton distribution visualization in perovskite nickelate devices utilizing nanofocused X-rays

We use a 30-nm x-ray beam to study the spatially resolved properties of a SmNiO$_3$-based nanodevice that is doped with protons. The x-ray absorption spectra supported by density-functional theory (DFT) simulations show partial reduction of nickel valence in the region with high proton concentration, which leads to the insulating behavior. Concurrently, x-ray diffraction reveals only a small lattice distortion in the doped regions. Together, our results directly show that the knob which proton doping modifies is the electronic valency, and not the crystal lattice. The studies are relevant to on-going efforts to disentangle structural and electronic effects across metal-insulator phase transitions in correlated oxides.

cond-mat.mtrl-sci↗

arXiv2021

Structural and Magnetic Transitions in the Planar Antiferromagnet Ba$_4$Ir$_3$O$_{10}$

We report the structural and magnetic ground state properties of the monoclinic compound barium iridium oxide Ba$_4$Ir$_3$O$_{10}$ using a combination of resonant x-ray scattering, magnetometry, and thermodynamic techniques. Magnetic susceptibility exhibits a pronounced antiferromagnetic transition at $T_{\text{N}}$ $\approx$ 25K, a weaker anomaly at $T_{\text{S}}$ $\approx$ 142K, and strong magnetic anisotropy at all temperatures. Resonant elastic x-ray scattering experiments reveal a second order structural phase transition at $T_{\text{S}}$ and a magnetic transition at $T_{\text{N}}$. Both structural and magnetic superlattice peaks are observed at $L$ = half integer values. The magnetization anomaly at $T_{\text{S}}$ implies the presence of magneto-elastic coupling, which conceivably facilitates the symmetry lowering. Mean field critical scattering is observed above $T_{\text{S}}$. The magnetic structure of the antiferromagnetic ground state is discussed based on the measured magnetic superlattice peak intensity. Our study not only presents essential information for understanding the intertwined structural and magnetic properties in Ba$_4$Ir$_3$O$_{10}$, but also highlights the necessary ingredients for exploring novel ground states with octahedra trimers.

cond-mat.str-el↗

arXiv2021

Charge ordering in superconducting copper oxides

Charge order has recently been identified as a leading competitor of high-temperature superconductivity in moderately doped cuprates. We provide a survey of universal and materials-specific aspects of this phenomenon, with emphasis on results obtained by scattering methods. In particular, we discuss the structure, periodicity, and stability range of the charge-ordered state, its response to various external perturbations, the influence of disorder, the coexistence and competition with superconductivity, as well as collective charge dynamics. In the context of this journal issue which honors Roger Cowley's legacy, we also discuss the connection of charge ordering with lattice vibrations and the central-peak phenomenon. We end the review with an outlook on research opportunities offered by new synthesis methods and experimental platforms, including cuprate thin films and superlattices.

cond-mat.str-el↗

arXiv2021

Magnon-spinon dichotomy in the Kitaev hyperhoneycomb $β$-Li$_2$IrO$_3$

The family of edge-sharing tri-coordinated iridates and ruthenates has emerged in recent years as a major platform for Kitaev spin liquid physics, where spins fractionalize into emergent magnetic fluxes and Majorana fermions with Dirac-like dispersions. While such exotic states are usually pre-empted by long-range magnetic order at low temperatures, signatures of Majorana fermions with long coherent times have been predicted to manifest at intermediate and higher energy scales, similar to the observation of spinons in quasi-1D spin chains. Here we present a Resonant Inelastic X-ray Scattering study of the magnetic excitations of the hyperhoneycomb iridate $β$-Li$_2$IrO$_3$ under a magnetic field with a record-high-resolution spectrometer. At low-temperatures, dispersing spin waves can be resolved around the predicted intertwined incommensurate spiral and field-induced zigzag orders, whose excitation energy reaches a maximum of 16meV. A 2T magnetic field softens the dispersion around ${\bf Q}=0$. The behavior of the spin waves under magnetic field is consistent with our semiclassical calculations for the ground state and the dynamical spin structure factor, which further predicts that the ensued intertwined uniform states remain robust up to very high fields (100 T). Most saliently, the low-energy magnon-like mode is superimposed by a broad continuum of excitations, centered around 35meV and extending up to 100meV. This high-energy continuum survives up to at least 300K -- well above the ordering temperature of 38K -- and gives evidence for pairs of long-lived Majorana fermions of the proximate Kitaev spin liquid.

cond-mat.str-el↗

arXiv2020

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↗

arXiv2020

Short-range nematic fluctuations in Sr1-xNaxFe2As2 superconductors

Interactions between nematic fluctuations, magnetic order and superconductivity are central to the physics of iron-based superconductors. Here we report on in-plane transverse acoustic phonons in hole-doped Sr$_{1-x}$Na$_x$Fe$_2$As$_2$ measured via inelastic X-ray scattering, and extract both the nematic susceptibility and the nematic correlation length. By a self-contained method of analysis, for the underdoped ($x=0.36$) sample, which harbors a magnetically-ordered tetragonal phase, we find it hosts a short nematic correlation length $ξ$ ~ 10 $Å$ and a large nematic susceptibility $χ_{\rm nem}$. The optimal-doped ($x=0.55$) sample exhibits weaker phonon softening effects, indicative of both reduced $ξ$ and $χ_{\rm nem}$. Our results suggest short-range nematic fluctuations may favor superconductivity, placing emphasis on the nematic correlation length for understanding the iron-based superconductors.

cond-mat.supr-con↗

arXiv2020

A hybrid optoelectronic Mott insulator

The coupling of electronic degrees of freedom in materials to create hybridized functionalities is a holy grail of modern condensed matter physics that may produce novel mechanisms of control. Correlated electron systems often exhibit coupled degrees of freedom with a high degree of tunability which sometimes lead to hybridized functionalities based on external stimuli. However, the mechanisms of tunability and the sensitivity to external stimuli are determined by intrinsic material properties which are not always controllable. A Mott metal-insulator transition, which is technologically attractive due to the large changes in resistance, can be tuned by doping, strain, electric fields, and orbital occupancy but cannot be, in and of itself, controlled externally with light. Here we present a new approach to produce hybridized functionalities using a properly engineered photoconductor/strongly-correlated hybrid heterostructure, showing control of the Metal-to-Insulator transition (MIT) using optical means. This approach combines a photoconductor, which does not exhibit an MIT, with a strongly correlated oxide, which is not photoconducting. Due to the close proximity between the two materials, the heterostructure exhibits large volatile and nonvolatile, photoinduced resistivity changes and substantial photoinduced shifts in the MIT transition temperatures. This approach can potentially be extended to other judiciously chosen combinations of strongly correlated materials with systems which exhibit optically, electrically or magnetically controllable behavior.

physics.app-ph↗

arXiv2019

Hidden spin-orbital order in the Kitaev hyperhoneycomb $β$-Li$_2$IrO$_3$

We report the existence of a phase transition at high temperature in the 3D Kitaev candidate material, $β$-Li$_2$IrO$_3$. We show that the transition is bulk, intrinsic and orders a tiny magnetic moment with a spatially anisotropic saturation moment. We show that even though this transition is global, it does not freeze the local Ir moments, which order at much lower temperatures into an incommensurate state. Rather, the ordered moment has an orbital origin that is coupled to spin correlations, likely of a Kitaev origin. The separate ordering of spin-correlated orbital moments and of local Ir moments reveals a novel way in which magnetic frustration in Kitaev systems can lead to coexisting magnetic states.

cond-mat.str-el↗

arXiv2019

Control of dopant crystallinity in electrochemically treated cuprate thin films

We present a methodology based on \textit{ex-situ} (post-growth) electrochemistry to control the oxygen concentration in thin films of the superconducting oxide La$_2$CuO$_{4+y}$ grown epitaxially on substrates of isostructural LaSrAlO$_4$. The superconducting transition temperature, which depends on the oxygen concentration, can be tuned by adjusting the pH level of the base solution used for the electrochemical reaction. As our main finding, we demonstrate that the dopant oxygens can either occupy the interstitial layer in an orientationally disordered state or organize into a crystalline phase via a mechanism in which dopant oxygens are inserted into the substrate, changing the lattice symmetry of both the substrate and the epitaxial film. We discuss this mechanism, and describe the resulting methodology as a platform to be explored in thin films of other transition metal oxides.

cond-mat.mtrl-sci↗

arXiv2019

Evolution of charge order topology across a magnetic phase transition in cuprate superconductors

Charge order is now accepted as an integral constituent of cuprate high-temperature superconductors, one that is intimately related to other instabilities in the phase diagram including antiferromagnetism and superconductivity. Unlike nesting-induced Peierls-like density waves, the charge correlations in the CuO2 planes have been predicted to display a rich momentum space topology depending on the detailed fermiology of the system. However, to date charge order has only been observed along the high-symmetry Cu-O bond directions. Here, using resonant soft X-ray scattering, we investigate the evolution of the full momentum space topology of charge correlations in Ln2CuO4 (Ln=Nd, Pr) as a function of intrinsic electron doping. We report that, upon electron doping the parent Mott insulator, charge correlations first emerge in a hitherto-unobserved form, with full (Cinf) rotational symmetry in momentum-space. At higher doping levels, the orientation of charge correlations is sharply locked to the Cu-O bond high-symmetry directions, restoring a more conventional bidirectional charge order with enhanced correlation lengths. Through charge susceptibility calculations, we closely reproduce the drastic evolution in the topology of charge correlations across an antiferromagnetic quantum phase transition, highlighting the interplay between spin and charge degrees of freedom in electron-doped cuprates. Finally, using the established link between charge correlations and the underlying fermiology, we propose a revised phase diagram of Ln2CuO4 with a superconducting region extending toward the Mott limit.

cond-mat.str-el↗

arXiv2019

Complex magnetic order in nickelate slabs

Magnetic ordering phenomena have a profound influence on the macroscopic properties of correlated-electron materials, but their realistic prediction remains a formidable challenge. An archetypical example is the ternary nickel oxide system RNiO3 (R = rare earth), where the period-four magnetic order with proposals of collinear and non-collinear structures and the amplitude of magnetic moments on different Ni sublattices have been subjects of debate for decades. Here we introduce an elementary model system - NdNiO3 slabs embedded in a non-magnetic NdGaO3 matrix - and use polarized resonant x-ray scattering (RXS) to show that both collinear and non-collinear magnetic structures can be realized, depending on the slab thickness. The crossover between both spin structures is correctly predicted by density functional theory and can be qualitatively understood in a low-energy spin model. We further demonstrate that the amplitude ratio of magnetic moments in neighboring NiO6 octahedra can be accurately determined by RXS in combination with a correlated double cluster model. Targeted synthesis of model systems with controlled thickness and synergistic application of polarized RXS and ab-initio theory thus provide new perspectives for research on complex magnetism, in analogy to two-dimensional materials created by exfoliation.

cond-mat.str-el↗

arXiv2018

Persistent low-energy phonon broadening near the charge order $q$-vector in bilayer cuprate Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$

We report a persistent low-energy phonon broadening around $q_{B} \sim 0.28$ r.l.u. along the Cu-O bond direction in the high-$T_c$ cuprate Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ (Bi-2212). We show that such broadening exists both inside and outside the conventional charge density wave (CDW) phase, via temperature dependent measurements in both underdoped and heavily overdoped samples. Combining inelastic hard x-ray scattering, diffuse scattering, angle-resolved photoemission spectroscopy, and resonant soft x-ray scattering at the Cu $L_3$-edge, we exclude the presence of a CDW in the heavily overdoped Bi-2212 similar to that observed in the underdoped systems. Finally, we discuss the origin of such anisotropic low-energy phonon broadening, and its potential precursory role to the CDW phase in the underdoped region.

cond-mat.str-el↗

arXiv2017

Local orthorhombicity in the magnetic $C_4$ phase of the hole-doped iron-arsenide superconductor Sr$_{1-x}$Na$_{x}$Fe$_2$As$_2$

We report temperature-dependent pair distribution function measurements of Sr$_{1-x}$Na$_{x}$Fe$_2$As$_2$, an iron-based superconductor system that contains a magnetic phase with reentrant tetragonal symmetry, known as the magnetic $C_4$ phase. Quantitative refinements indicate that the instantaneous local structure in the $C_4$ phase is comprised of fluctuating orthorhombic regions with a length scale of $\sim$2 nm, despite the tetragonal symmetry of the average static structure. Additionally, local orthorhombic fluctuations exist on a similar length scale at temperatures well into the paramagnetic tetragonal phase. These results highlight the exceptionally large nematic susceptibility of iron-based superconductors and have significant implications for the magnetic $C_4$ phase and the neighboring $C_2$ and superconducting phases.

cond-mat.supr-con↗

arXiv2017

Field-induced intertwined orders in 3D Mott-Kitaev honeycomb $β$-Li2IrO3

Honeycomb iridates are thought to have strongly spin-anisotropic exchange interactions that could lead to an extraordinary state of matter known as the Kitaev quantum spin liquid. The realization of this state requires almost perfectly frustrated interactions between the magnetic Ir$^{4+}$ ions, but small imbalances in energy make other ordered states more favorable. Indeed, the closeness in energy of these ordered states is itself a signature of the intrinsic frustration in the system. In this work, we illustrate that small magnetic fields can be employed to drive the frustrated quantum magnet $β-$Li$_2$IrO$_3$,between different broken symmetry states, but without causing a true thermodynamic phase transition. This field-induced broken symmetry phase has all the signatures of a thermodynamic order parameter, but it is never truly formed in zero field. Rather, it is summoned when the scales of frustration are appropriately tipped, intertwined with other nearby quantum states.

cond-mat.str-el↗