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Mohamed Oudah

Publications and source records attributed to Mohamed Oudah.

At least 19 recordsLinked to original sources

Rare-earth oxysulfides RE$_2$O$_2$S as model mixed-anion frustrated magnets

The study of low-dimensional and anisotropic magnetism is a promising avenue for the discovery of novel quantum phenomena. Mixed-anion materials, defined by the coordination of metal cations by two or more distinct anionic species, provide an intrinsically anisotropic platform for the tuning of structural, magnetic, and electronic properties. In this work, we report the synthesis and characterization of a family of rare-earth oxysulfide (RE$_2$O$_2$S) antiferromagnets (AFM) possessing a triangular-bilayer slab lattice geometry. Long-range AFM order is observed for the majority of compositions, with several (RE = Ce, Pr, Nd, Sm) having been previously unreported. Although assumed to form stoichiometrically, pair distribution function (PDF) analysis provides evidence for significant, synthesis-dependent interslab structural disorder as RE$_2$O$_{2+x}$S$_{1-x}$, resulting in significant variability in the bulk magnetic response of the Nd member. This work highlights the tunability of frustrated magnetic ground states in rare-earth-based mixed-anion materials, and the importance of thorough structural characterization in the discovery of new mixed-anion magnets.

cond-mat.str-el

Visualizing Vortex Cluster Dynamics in the Weak Type-II Superconductor CaSb$_2$

Scanning SQUID imaging of CaSb$_2$ reveals dense vortex clusters with enhanced boundary susceptibility and suppressed internal vortex motion, which features inconsistent with both isolated vortex and flux tube behaviors. These measurements provide the first local visualization of magnetic dynamics within vortex clusters in a weakly pinned superconductor, offering a new route to probe non-monotonic vortex-vortex interactions that are typically expected in single-band type-II/1 or multiband type-1.5 superconductors. Although the superfluid density follows a single-gap BCS model and the Ginzburg-Landau parameter of CaSb$_2$ lies slightly outside the type-II/1 regime, vortex clustering and spatially inhomogeneous dynamics are clearly observed, indicating physics beyond existing microscopic theories for single-band superconductors.

cond-mat.supr-con

Direct Fabrication of a Superconducting Two-Dimensional Electron Gas on KTaO3(111) via Mg-Induced Surface Reduction

Two-dimensional electron gases (2DEGs) at the surfaces of KTaO3 have become an exciting platform for exploring strong spin-orbit coupling, Rashba physics, and low-carrier-density superconductivity. Yet, a large fraction of reported KTaO3-based 2DEGs has been realized through chemically complex overlayers that both generate carriers and can obscure the native electronic structure, making spectroscopic access to the underlying 2DEG challenging. Here, we demonstrate a simple and direct method to generate a superconducting 2DEG on KTaO3(111) using Mg-induced surface reduction in molecular-beam epitaxy (MBE). Mg has an extremely low sticking coefficient at elevated temperatures, enabling the formation of an ultrathin (less than 1-2 monolayers) MgO layer that is transparent to soft x-ray photoemission spectroscopy (XPS) and angle-resolved photoemission spectroscopy (ARPES). This allows direct measurement of the surface chemistry and low-energy electronic structure of the pristine reduced surface without the need for a several-nanometer-thick capping layer. XPS shows clear reduction of Ta5+ to lower oxidation states, while ARPES reveals a parabolic Ta 5d conduction band with an approximately 150 meV bandwidth and additional subband features arising from quantum confinement. Transport measurements confirm a superconducting transition below 0.7 K. Together, these results demonstrate a chemically straightforward and controllable pathway for fabricating spectroscopically accessible superconducting 2DEGs on KTaO3(111), and provide a powerful new platform for investigating the mechanisms underlying orientation-dependent superconductivity in KTaO3-based oxide interfaces.

cond-mat.supr-con

Kramers nodal lines in intercalated TaS$_2$ superconductors

Kramers degeneracy is one fundamental embodiment of the quantum mechanical nature of particles with half-integer spin under time reversal symmetry. Under the chiral and noncentrosymmetric achiral crystalline symmetries, Kramers degeneracy emerges respectively as topological quasiparticles of Weyl fermions and Kramers nodal lines (KNLs), anchoring the Berry phase-related physics of electrons. However, an experimental demonstration for ideal KNLs well isolated at the Fermi level is lacking. Here, we establish a class of noncentrosymmetric achiral intercalated transition metal dichalcogenide superconductors with large Ising-type spin-orbit coupling, represented by In$_x$TaS$_2$, to host an ideal KNL phase. We provide evidence from angle-resolved photoemission spectroscopy with spin resolution, angle-dependent quantum oscillation measurements, and ab-initio calculations. Our work not only provides a realistic platform for realizing and tuning KNLs in layered materials, but also paves the way for exploring the interplay between KNLs and superconductivity, as well as applications pertaining to spintronics, valleytronics, and nonlinear transport.

cond-mat.supr-con

Highly Uniform Magnetic and Electronic Environment in Non-Centrosymmetric Superconductor LaRhGe$_3$

We report the results of $^{139}$La NMR measurements in the non-centrosymmetric superconductor LaRhGe$_3$. This material crystallizes in a tetragonal structure without inversion symmetry and exhibits type-I superconductivity below 385 mK. We observed remarkably sharp NMR signals, indicating that the magnetic and electronic properties of the sample are extremely uniform in LaRhGe$_3$ despite the complex crystal structure. Our NMR results indicate that LaRhGe$_3$ is a weakly correlated semimetal in the normal state.

cond-mat.supr-con

Using $k$-means to sort spectra: electronic order mapping from scanning tunneling spectroscopy measurements

Hyperspectral imaging techniques have a unique ability to probe the inhomogeneity of material properties whether driven by compositional variation or other forms of phase segregation. In the doped cuprates, iridates, and related materials, scanning tunneling microscopy/spectroscopy (STM/STS) measurements have found the emergence of pseudogap 'puddles' from the macroscopically Mott insulating phase with increased doping. However, categorizing this hyperspectral data by electronic order is not trivial, and has often been done with ad hoc methods. In this paper we demonstrate the utility of $k$-means, a simple and easy-to-use unsupervised clustering method, as a tool for classifying heterogeneous scanning tunneling spectroscopy data by electronic order for Rh-doped Sr$_2$IrO$_{4}$, a cuprate-like material. Applied to STM data acquired within the Mott phase, $k$-means successfully identified areas of Mott order and of pseudogap order. The unsupervised nature of $k$-means limits avenues for bias, and provides clustered spectral shapes without a priori knowledge of the physics. Additionally, we demonstrate successful use of $k$-means as a preprocessing tool to constrain phenomenological function fitting. Clustering the data allows us to reduce the fitting parameter space, limiting over-fitting. We suggest $k$-means as a fast, simple model for processing hyperspectral data on materials of mixed electronic order.

cond-mat.str-el

Effect of high pressure synthesis conditions on the formation of high entropy oxides

High entropy materials are often entropy stabilized, meaning that the configurational entropy from multiple elements sharing a single lattice site stabilizes the structure. In this work, we study how high-pressure synthesis conditions can stabilize or destabilize a high entropy oxide (HEO). We study the high-pressure and high-temperature phase equilibria of two well-known families of HEOs: the rock-salt structured compound (Mg,Co,Ni,Cu,Zn)O including some cation substitutions and the spinel structured (Cr,Mn,Fe,Co,Ni)$_3$O$_4$. Syntheses were performed at various temperatures, pressures, and oxygen activity levels resulting in dramatically different synthesis outcomes. In particular, in the rock salt HEO we observe the competing tenorite and wurtzite phases and the possible formation of a layered rock salt phase, while the spinel HEO is highly susceptible to decomposition into a mixture of rock-salt and corundum phases. At the highest tested pressures, 15 GPa, we discover the transformation of the spinel HEO into a metastable modified ludwigite-type structure with nominal formula (Cr,Mn,Fe,Co,Ni)$_4$O$_5$. The relationship between the synthesis conditions and the final reaction product is not straightforward. Nonetheless, we conclude that high-pressure conditions provide an important opportunity to synthesize high entropy phases that cannot be formed any other way.

cond-mat.mtrl-sci

Discovery of Superconductivity and Electron-Phonon Drag in the Non-Centrosymmetric Weyl Semimetal LaRhGe$_3$

We present an exploration of the effect of electron-phonon coupling and broken inversion symmetry on the electronic and thermal properties of the semimetal LaRhGe$_3$. Our transport measurements reveal evidence for electron-hole compensation at low temperatures, resulting in a large magnetoresistance of 3000% at 1.8 K and 14 T. The carrier concentration is on the order of $10^{21}\rm{/cm}^3$ with high carrier mobilities of $2000~\rm{cm}^2/\rm{Vs}$. When coupled to our theoretical demonstration of symmetry-protected $\textit{almost movable}$ Weyl nodal lines, we conclude that LaRhGe$_3$ supports a Weyl semimetallic state. We discover superconductivity in this compound with a $T_{\text c}$ of 0.39(1) K and $B_{\rm{c}}(0)$ of 2.2(1) mT, with evidence from specific heat and transverse-field muon spin relaxation. We find an exponential dependence in the normal state electrical resistivity below $\sim50$ K, while Seebeck coefficient and thermal conductivity measurements each reveal a prominent peak at low temperatures, indicative of strong electron-phonon interactions. To this end, we examine the temperature-dependent Raman spectra of LaRhGe$_3$ and find that the lifetime of the lowest energy $A_1$ phonon is dominated by phonon-electron scattering instead of anharmonic decay. We conclude that LaRhGe$_3$ has strong electron-phonon coupling in the normal state, while the superconductivity emerges from weak electron-phonon coupling. These results open up the investigation of electron-phonon interactions in the normal state of superconducting non-centrosymmetric Weyl semimetals.

cond-mat.supr-con

Physical properties and electronic structure of the two-gap superconductor V$_{2}$Ga$_{5}$

We present a thorough investigation of the physical properties and superconductivity of the binary intermetallic V2Ga5. Electrical resistivity and specific heat measurements show that V2Ga5 enters its superconducting state below Tsc = 3.5 K, with a critical field of Hc2,perp c(Hc2,para c) = 6.5(4.1) kOe. With H perp c, the peak effect was observed in resistivity measurements, indicating the ultrahigh quality of the single crystal studied. The resistivity measurements under high pressure reveal that the Tsc is suppressed linearly with pressure and reaches absolute zero around 20 GPa. Specific heat and muon spin relaxation measurements both indicate that the two-gap s-wave model best describes the superconductivity of V2Ga5. The spectra obtained from angle-resolved photoemission spectroscopy measurements suggest that two superconducting gaps open at the Fermi surface around the Z and Γ points. These results are verified by first-principles band structure calculations. We therefore conclude that V2Ga5 is a phonon-mediated two-gap s-wave superconductor

cond-mat.supr-con

Ion-Implanted $^8$Li Nuclear Magnetic Resonance in Highly Oriented Pyrolytic Graphite

We report $β$-detected nuclear magnetic resonance of ultra-dilute $^{8}$Li$^{+}$ implanted in highly oriented pyrolytic graphite (HOPG). The absence of motional narrowing and diffusional spin-lattice relaxation implies Li$^+$ is not appreciably mobile up to 400 K, in sharp contrast to the highly lithiated stage compounds. However, the relaxation is remarkably fast and persists down to cryogenic temperatures. Ruling out extrinsic paramagnetic impurities and intrinsic ferromagnetism, we conclude the relaxation is due to paramagnetic centers correlated with implantation. While the resulting effects are not consistent with a Kondo impurity, they also differ from free paramagnetic centers, and we suggest that a resonant scattering approach may account for much of the observed phenomenology.

cond-mat.mtrl-sci

Phase stability of entropy stabilized oxides with the $α$-PbO$_2$ structure

The prediction of new high entropy oxides (HEOs) remains a profound challenge due to their inherent chemical complexity. In this work, we combine experimental and computational methods to search for new HEOs in the tetravalent $A$O$_2$ family, using exclusively $d^0$ and $d^{10}$ cations, and to explain the observed phase stability of the $α$-PbO$_2$ structure, as found for the medium entropy oxide (Ti, Zr, Hf, Sn)O$_2$. Using a pairwise approach to approximate the mixing enthalpy, we confirm that $α$-PbO$_2$ is the expected lowest energy structure for this material above other candidates including rutile, baddeleyite, and fluorite structures. We also show that no other five-component compound composed of the tetravalent cations considered here is expected to form under solid state synthesis conditions, which we verify experimentally. Ultimately, we conclude that the flexible geometry of the $α$-PbO$_2$ structure can be used to understand its stability among tetravalent HEOs.

cond-mat.mtrl-sci

Non-local electrodynamics in ultra-pure PdCoO$_{2}$

The motion of electrons in the vast majority of conductors is diffusive, obeying Ohm's law. However, the recent discovery and growth of high-purity materials with extremely long electronic mean free paths has sparked interest in non-ohmic alternatives, including viscous and ballistic flow. Although non-ohmic transport regimes have been discovered across a range of materials, including two-dimensional electron gases, graphene, topological semimetals, and the delafossite metals, determining their nature has proved to be challenging. Here, we report on a new approach to the problem, employing broadband microwave spectroscopy of the delafossite metal PdCoO$_{2}$ in three distinct sample geometries that would be identical for diffusive transport. The observed differences, which go as far as differing power laws, take advantage of the hexagonal symmetry of PdCoO$_{2}$. This permits a particularly elegant symmetry-based diagnostic for non-local electrodynamics, with the result favouring ballistic over strictly hydrodynamic flow. Furthermore, it uncovers a new effect for ballistic electron flow, owing to the highly facetted shape of the hexagonal Fermi surface. We combine our extensive dataset with an analysis of the Boltzmann equation to characterize the non-local regime in PdCoO$_{2}$. More broadly, our results highlight the potential of broadband microwave spectroscopy to play a central role in investigating exotic transport regimes in the new generation of ultra-high conductivity materials.

cond-mat.mes-hall

Understanding the role of entropy in high entropy oxides

The field of high entropy oxides (HEOs) flips traditional materials science paradigms on their head by seeking to understand what properties arise in the presence of profound configurational disorder. This disorder, which originates from multiple elements sharing a single lattice site, can take on a kaleidoscopic character due to the vast numbers of possible elemental combinations. High configurational disorder appears to imbue some HEOs with functional properties that far surpass their non-disordered analogs. While experimental discoveries abound, efforts to characterize the true magnitude of the configurational entropy and understand its role in stabilizing new phases and generating superior functional properties have lagged behind. Understanding the role of configurational disorder in existing HEOs is the crucial link to unlocking the rational design of new HEOs with targeted properties. In this Perspective, we attempt to establish a framework for articulating and beginning to address these questions in pursuit of a deeper understanding of the true role of entropy in HEOs.

cond-mat.mtrl-sci

Entropy engineering and tunable magnetic order in the spinel high entropy oxide

Spinel oxides are an ideal setting to explore the interplay between configurational entropy, site selectivity, and magnetism in high entropy oxides. In this work we characterize the magnetic properties of the spinel (Cr,Mn,Fe,Co,Ni)$_3$O$_4$ and study the evolution of its magnetism as a function of non-magnetic gallium substitution. Across the range of compositions studied here, from 0% to 40% Ga, magnetic susceptibility and powder neutron diffraction measurements show that ferrimagnetic order is robust in the spinel HEO. However, we also find that the ferrimagnetic order is highly tunable, with the ordering temperature, saturated and sublattice moments, and magnetic hardness all varying significantly as a function of Ga concentration. Through x-ray absorption and magnetic circular dichroism, we are able to correlate this magnetic tunability with strong site selectivity between the various cations and the tetrahedral and octahedral sites in the spinel structure. In particular, we find that while Ni and Cr are largely unaffected by the substitution with Ga, the occupancies of Mn, Co, and Fe are each significantly redistributed. Ga substitution also requires an overall reduction in the transition metal valence, and this is entirely accommodated by Mn. Finally, we show that while site selectivity has an overall suppressing effect on the configurational entropy, over a certain range of compositions, Ga substitution yields a striking increase in the configurational entropy and may confer additional stabilization. Spinel oxides can be tuned seamlessly from the low-entropy to the high-entropy regime, making this an ideal platform for entropy engineering.

cond-mat.mtrl-sci

Quasiparticle interference observation of the topologically non-trivial drumhead surface state in ZrSiTe

Drumhead surface states that link together loops of nodal lines arise in Dirac nodal-line semimetals as a consequence of the topologically non-trivial band crossings. We used low-temperature scanning tunneling microscopy and Fourier-transformed scanning tunneling spectroscopy to investigate the quasiparticle interference (QPI) properties of ZrSiTe. Our results show two scattering signals across the drumhead state resolving the energy-momentum relationship through the occupied and unoccupied energy ranges it is predicted to span. Observation of this drumhead state is in contrast to previous studies on ZrSiS and ZrSiSe, where the QPI was dominated by topologically trivial bulk bands and surface states. Furthermore, we observe a near $\mathbf{k} \rightarrow -\mathbf{k}$ scattering process across the $Γ$-point, enabled by scattering between the spin-split drumhead bands in this material.

cond-mat.mtrl-sci

Discovery of Superconductivity in (Ba,K)SbO$_{3}$

Superconducting bismuthates (Ba,K)BiO$_{3}$ (BKBO) constitute an interesting class of superconductors in that superconductivity with a remarkably high $T_\mathrm{c}$ of 30 K arises in proximity to charge density wave (CDW) order. Prior understanding on the driving mechanism of the CDW and superconductivity emphasizes the role of either bismuth (negative $U$ model) or oxygen ions (ligand hole model). While holes in BKBO presumably reside on oxygen owing to their negative charge transfer energy, so far there has been no other comparative material studied. Here, we introduce (Ba,K)SbO$_{3}$ (BKSO) in which the Sb 5$s$ orbital energy is higher than that of the Bi 6$s$ orbitals enabling tuning of the charge transfer energy from negative to slightly positive. The parent compound BaSbO$_{3-δ}$ shows a larger CDW gap compared to the undoped bismuthate BaBiO$_{3}$. As the CDW order is suppressed via potassium substitution up to 65 %, superconductivity emerges, rising up to $T_\mathrm{c}$ = 15 K. This value is lower than the maximum $T_\mathrm{c}$ of BKBO, but higher by more than a factor of two at comparable potassium concentrations. The discovery of an enhanced CDW gap and superconductivity in BKSO indicates that the sign of the charge transfer energy may not be crucial, but instead strong metal-oxygen covalency plays the essential role in constituting a CDW and high-$T_\mathrm{c}$ superconductivity in the main-group perovskite oxides.

cond-mat.supr-con

Electronic Structure of the Bond Disproportionated Bismuthate Ag$_2$BiO$_3$

We present a comprehensive study on the silver bismuthate Ag$_2$BiO$_3$, synthesized under high-pressure high-temperature conditions, which has been the subject of recent theoretical work on topologically complex electronic states. We present X-ray photoelectron spectroscopy results showing two different bismuth states, and X-ray absorption spectroscopy results on the oxygen $K$-edge showing holes in the oxygen bands. These results support a bond disproportionated state with holes on the oxygen atoms for Ag$_2$BiO$_3$. We estimate a band gap of $\sim$1.25~eV for Ag$_2$BiO$_3$ from optical conductivity measurements, which matches the band gap in density functional calculations of the electronic band structure in the non-symmorphic space group $Pnn2$, which supports two inequivalent Bi sites. In our band structure calculations the disproportionated Ag$_2$BiO$_3$ is expected to host Weyl nodal chains, one of which is located $\sim$0.5~eV below the Fermi level. Furthermore, we highlight similarities between Ag$_2$BiO$_3$ and the well-known disproportionated bismuthate BaBiO$_3$, including breathing phonon modes with similar energy. In both compounds hybridization of Bi-$6s$ and O-$2p$ atomic orbitals is important in shaping the band structure, but in contrast to the Ba-$5p$ in BaBiO$_3$, the Ag-$4d$ bands in Ag$_2$BiO$_3$ extend up to the Fermi level.

cond-mat.mtrl-sci

Signature of an Ultrafast Photo-Induced Lifshitz Transition in the Nodal-Line Semimetal ZrSiTe

Here we report an ultrafast optical spectroscopic study of the nodal-line semimetal ZrSiTe. Our measurements reveal that, converse to other compounds of the family, the sudden injection of electronic excitations results in a strongly coherent response of an $A_{1g}$ phonon mode which dynamically modifies the distance between Zr and Te atoms and Si layers. "Frozen phonon" DFT calculations, in which band structures are calculated as a function of nuclear position along the phonon mode coordinate, show that large displacements along this mode alter the material's electronic structure significantly, forcing bands to approach and even cross the Fermi energy. The incoherent part of the time domain response reveals that a delayed electronic response at low fluence discontinuously evolves into an instantaneous one for excitation densities larger than $3.43 \times 10^{17}$ cm$^{-3}$. This sudden change of the dissipative channels for electronic excitations is indicative of an ultrafast Lifshitz transition which we tentatively associate to a change in topology of the Fermi surface driven by a symmetry preserving $A_{1g}$ phonon mode.

cond-mat.mtrl-sci