arXiv subjects

A. Said

Publications and source records attributed to A. Said.

14 recordsLinked to original sources

arXiv2024

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↗

arXiv2024

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↗

arXiv2021

Divergence of Majorana-Phonon Scattering in Kitaev Quantum Spin Liquid

Magnetoelastic interaction couples spin and lattice degrees of freedom and plays a key role in thermal transport properties of magnetic insulators. In the Kitaev quantum spin liquid, the low energy excitations are charge neutral Majorana fermions, which transform the magnetoelasctic interaction into Majorana-phonon scattering. Motivated by anomalous thermal properties of the Kitaev quantum spin liquid candidate RuCl$_3$, in this letter, we combine meV resolution inelastic x-ray scattering and theoretical calculation to examine the Majorana-phonon scattering. We analytically derive the velocity-dependent Majorana-phonon scattering and find a divergence when the acoustic phonons and the itinerant Majorana fermions have the same velocity. Based on the experimentally determined acoustic phonon velocity in RuCl$_3$, we estimate the range in the Kitaev interaction for which divergent Majorana-phonon scattering can happen. Our result opens a new avenue to uncover fractionalized quasiparticles in the Kitaev quantum spin liquid and emphasizes the critical role of lattice excitations in RuCl$_3$.

cond-mat.str-el↗

arXiv2021

Spatial symmetry constraint of charge-ordered kagome superconductor CsV$_3$Sb$_5$

Elucidating the symmetry of intertwined orders in exotic superconductors is at the quantum frontier. Recent surface sensitive studies of the topological kagome superconductor CsV$_3$Sb$_5$ discovered a cascade 4a$_0$ superlattice below the charge density wave (CDW) ordering temperature, which can be related to the pair density modulations in the superconducting state. If the 4a$_0$ phase is a bulk and intrinsic property of the kagome lattice, this would form a striking analogy to the stripe order and pair density wave discovered in the cuprate high-temperature superconductors, and the cascade ordering found in twisted bilayer graphene. High-resolution X-ray diffraction has recently been established as an ultra-sensitive probe for bulk translational symmetry-breaking orders, even for short-range orders at the diffusive limit. Here, combining high-resolution X-ray diffraction, scanning tunneling microscopy and scanning transmission electron microscopy, we demonstrate that the 4a$_0$ superstructure emerges uniquely on the surface and hence exclude the 4a$_0$ phase as the origin of any bulk transport or spectroscopic anomaly. Crucially, we show that our detected 2$\times$2$\times$2 CDW order breaks the bulk rotational symmetry to C2, which can be the driver for the bulk nematic orders and nematic surface superlattices including the 4a$_0$ phase. Our high-resolution data impose decisive spatial symmetry constraints on emergent electronic orders in the kagome superconductor CsV$_3$Sb$_5$.

cond-mat.mtrl-sci↗

arXiv2021

Geometry of the charge density wave in kagom${\'e}$ metal AV$_{3}$Sb$_{5}$

Kagom${\'e}$ lattice is a fertile platform for topological and intertwined electronic excitations. Recently, experimental evidence of an unconventional charge density wave (CDW) is observed in a Z2 kagom${\'e}$ metal AV$_{3}$Sb$_{5}$ (A= K, Cs, Rb). This observation triggers wide interests on the interplay between frustrated crystal structure and Fermi surface instabilities. Here we analyze the lattice effect and its impact on CDW in AV$_{3}$Sb$_{5}$. Based on published experimental data, we show that the CDW induced structural distortions is consistent with the theoretically predicted inverse star-of-David pattern, which preserves the $D_{6h}$ symmetry in the kagom${\'e}$ plane but breaks the sixfold rotational symmetry of the crystal due to the phase shift between kagom${\'e}$ layers. The coupling between the lattice and electronic degrees of freedom yields a weak first order structural transition without continuous change of lattice dynamics. Our result emphasizes the fundamental role of lattice geometry in proper understanding of unconventional electronic orders in AV$_{3}$Sb$_{5}$.

cond-mat.str-el↗

arXiv2021

Observation of Unconventional Charge Density Wave without Acoustic Phonon Anomaly in Kagome Superconductors AV3Sb5 (A=Rb,Cs)

The combination of non-trivial band topology and symmetry breaking phases gives rise to novel quantum states and phenomena such as topological superconductivity, quantum anomalous Hall effect and axion electrodynamics. Evidence of intertwined charge density wave (CDW) and superconducting order parameters has recently been observed in a novel kagome material AV3Sb5 (A=K,Rb,Cs) that features a Z2 topological invariant in the electronic structure. However, the origin of the CDW and its intricate interplay with topological state has yet to be determined. Here, using hard x-ray scattering, we demonstrate a three-dimensional (3D) CDW with 2*2*2 superstructure in (Rb,Cs)V3Sb5. Unexpectedly, we find that the CDW fails to induce acoustic phonon anomalies at the CDW wavevector but yields a novel Raman mode which quickly damps into a broad continuum below the CDW transition temperature. Our observations exclude strong electron-phonon coupling driven CDW in AV3Sb5 and point to an unconventional and electronic-driven mechanism that couples the CDW and the topological band structure.

cond-mat.supr-con↗

arXiv2020

Giant Phonon Anomalies in the Proximate Kitaev Quantum Spin Liquid $\alpha$-RuCl$_3$

The Kitaev quantum spin liquid epitomizes an entangled topological state, for which two flavors of fractionalized low-energy excitations are predicted: the itinerant Majorana fermion and the Z2 gauge flux. Detection of these excitations remains challenging, because of their fractional quantum numbers and non-locality. It was proposed recently that fingerprints of fractional excitations are encoded in the phonon spectra of Kitaev quantum spin liquids through a novel fractional-excitation-phonon coupling. Here, we uncover this effect in $\alpha$-RuCl3 using inelastic X-ray scattering with meV resolution. At high temperature, we discover interlaced optical phonons intercepting a transverse acoustic phonon between 3 and 7 meV. Upon decreasing temperature, the optical phonons display a large intensity enhancement near the Kitaev energy, JK~8 meV, that coincides with a giant acoustic phonon softening near the Z2 gauge flux energy scale. This fractional excitation induced phonon anomalies uncover the key ingredient of the quantum thermal Hall effect in $\alpha$-RuCl3 and demonstrates a proof-of-principle method to detect fractional excitations in topological quantum materials.

cond-mat.str-el↗

arXiv2020

Observation of a Chiral Wave Function in Twofold Degenerate Quadruple Weyl System BaPtGe

Topological states in quantum materials are defined by non-trivial topological invariants, such as the Chern number, which are properties of their bulk wave functions. A remarkable consequence of topological wave functions is the emergence of edge modes, a phenomenon known as bulk-edge correspondence, that gives rise to quantized or chiral physical properties. While edge modes are widely presented as signatures of non-trivial topology, how bulk wave functions can manifest explicitly topological properties remains unresolved. Here, using high-resolution inelastic x-ray spectroscopy (IXS) combined with first principles calculations, we report experimental signatures of chiral wave functions in the bulk phonon spectrum of BaPtGe, which we show to host a previously undiscovered twofold degenerate quadruple Weyl node. The chirality of the degenerate phononic wave function yields a non-trivial phonon dynamical structure factor, S(Q,$\omega$), along high-symmetry directions, that is in excellent agreement with numerical and model calculations. Our results establish IXS as a powerful tool to uncover topological wave functions, providing a key missing ingredient in the study of topological quantum matter.

cond-mat.mtrl-sci↗

arXiv2020

Instrumentation for high-resolution laser spectroscopy at the ALTO radioactive-beam facility

Collinear laser spectroscopy is one of the essential tools for nuclear-structure studies. It allows nuclear electromagnetic properties of ground and isomeric states to be extracted with high experimental precision. Radioactive-beam facilities worldwide strive to introduce such capabilities or to improve existing ones. Here we present the implementation of collinear laser spectroscopy at the ALTO research laboratory, along with data from successful off-line commissioning using sodium beam. The instrumental constituents are discussed with emphasis on simple technical solutions and maximized use of standard equipment. Potential future applications are outlined.

physics.ins-det↗

arXiv2018

Pseudospin-lattice coupling in the spin-orbit Mott insulator Sr2IrO4

Spin-orbit entangled magnetic dipoles, often referred to as pseudospins, provide a new avenue to explore novel magnetism inconceivable in the weak spin-orbit coupling limit, but the nature of their low-energy interactions remains to be understood. We present a comprehensive study of the static magnetism and low-energy pseudospin dynamics in the archetypal spin-orbit Mott insulator Sr2IrO4. We find that in order to understand even basic magnetization measurements, a formerly overlooked in-plane anisotropy is fundamental. In addition to magnetometry, we use neutron diffraction, inelastic neutron scattering and resonant elastic and inelastic x-ray scattering to identify and quantify the interactions that determine the global symmetry of the system and govern the linear responses of pseudospins to external magnetic felds and their low-energy dynamics. We find that a pseudospin-only Hamiltonian is insufficient for an accurate description of the magnetism in Sr2IrO4 and that pseudospin-lattice coupling is essential. This finding should be generally applicable to other pseudospin systems with sizable orbital moments sensitive to anisotropic crystalline environments.

cond-mat.str-el↗

arXiv2016

Engineering One-Dimensional Quantum Stripes from Superlattices of Two-Dimensional Layered Materials

One-dimensional (1D) quantum systems, which are predicted to exhibit novel states of matter in theory, have been elusive in experiment. Here we report a superlattice method of creating artificial 1D quantum stripes, which offers dimensional tunability from two- to one-dimensions. As a model system, we have fabricated 1D iridium (Ir) stripes using a-axis oriented superlattices of a relativistic Mott insulator Sr2IrO4 and a wide bandgap insulator LaSrGaO4, both of which are crystals with layered structure. In addition to the successful formation of 1D Ir-stripe structure, we have observed 1D quantum-confined electronic states from optical spectroscopy and resonant inelastic x-ray scattering. Since this 1D superlattice approach can be applied to a wide range of layered materials, it opens a new era of 1D science.

cond-mat.mtrl-sci↗

arXiv2013

Ferromagnetic Exchange Anisotropy from Antiferromagnetic Superexchange in the Mixed 3d-5d Transition-Metal Compound Sr3CuIrO6

We report a combined experimental and theoretical study of the unusual ferromagnetism in the one-dimensional copper-iridium oxide Sr$_3$CuIrO$_6$. Utilizing Ir $L_3$ edge resonant inelastic x-ray scattering, we reveal a large gap magnetic excitation spectrum. We find that it is caused by an unusual exchange anisotropy generating mechanism, namely, strong ferromagnetic anisotropy arising from antiferromagnetic superexchange, driven by the alternating strong and weak spin-orbit coupling on the $5d$ Ir and 3d Cu magnetic ions, respectively. From symmetry consideration, this novel mechanism is generally present in systems with edge-sharing Cu$^{2+}$O$_4$ plaquettes and Ir$^{4+}$O$_6$ octahedra. Our results point to unusual magnetic behavior to be expected in mixed 3d-5d transition-metal compounds via exchange pathways that are absent in pure 3d or 5d compounds.

cond-mat.str-el↗

arXiv2012

Testing the validity of the strong spin-orbit-coupling limit for octahedrally coordinated iridates in a model system Sr$_3$CuIrO$_6$

The electronic structure of Sr$_3$CuIrO$_6$, a model system for the 5d Ir ion in an octahedral environment, is studied through a combination of resonant inelastic x-ray scattering (RIXS) and theoretical calculations. RIXS spectra at the Ir L$_3$-edge reveal an Ir $t_{2g}$ manifold that is split into three levels, in contrast to the expectations of the strong spin-orbit-coupling limit. Effective Hamiltonian and $ab inito$ quantum chemistry calculations find a strikingly large non-cubic crystal field splitting comparable to the spin-orbit coupling, which results in a strong mixing of the $j_{\mathsf{eff}}=1/2$ and $j_{\mathsf{eff}}=3/2$ states and modifies the isotropic wavefunctions on which many theoretical models are based.

cond-mat.str-el↗

arXiv2008

X-ray Studies of Structure and Defects in Solid 4He from 50 mK to Melting

Recent measurements have found non-classical rotational inertia (NCRI) in solid 4He starting at T ~ 200 mK, leading to speculation that a supersolid state may exist in these materials. Differences in the NCRI fraction due to the growth method and annealing history imply that defects play an important role in the effect. Using x-ray synchrotron radiation, we have studied the nature of the crystals and the properties of the defects in solid 4He at temperatures down to 50 mK. Measurements of peak intensities and lattice parameters do not show indications of the supersolid transition. Using growth methods similar to those of groups measuring the NCRI we find that large crystals form. Scanning with a small (down to 10 x 10 um2) beam, we resolve a mosaic structure within these crystals consistent with numerous small angle grain boundaries. The mosaic shows significant shifts over time even at temperatures far from melting. We discuss the relevance of these defects to the NCRI observations.

cond-mat.other↗