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The discovery of superconductivity in planar nickelates raises the question of how the electronic structure and correlations of Ni 1+ compounds compare to those of the Cu 2+ cuprate superconductors. Here, we present an angle-resolved photoemission spectroscopy (ARPES) study of the trilayer nickelate Pr 4 Ni 3 O 8 , revealing a Fermi surface resembling that of the hole-doped cuprates but with critical differences. Specifically, the main portions of the Fermi surface are extremely similar to that of the bilayer cuprates, with an additional piece that can accommodate additional hole doping. We find that the electronic correlations are about twice as strong in the nickelates and are almost k -independent, indicating that they originate from a local effect, likely the Mott interaction, whereas cuprate interactions are somewhat less local. Nevertheless, the nickelates still demonstrate the strange-metal behavior in the electron scattering rates. Understanding the similarities and differences between these two families of strongly correlated superconductors is an important challenge.

We report the synthesis and characterization of phase pure Ta3Sb, a material predicted to be topological with eightfold degenerate fermionic states [Science 353, aaf5037 (2016)] and to exhibit a large spin Hall effect [Sci. Adv. 5, eaav8575 (2019]. We observe superconductivity in Ta3Sb with Tc~ 0.67 K in both electrical resistivity \r{ho}(T) and specific heat C(T) measurements. Field dependent measurements yield the superconducting phase diagram with an upper critical field of Hc2(0) ~ 0.95 T, corresponding to a superconducting coherence length of {\xi} ~18.6 nm. The gap ratio deduced from specific heat anomaly, 2{\Delta}0/kBTc is 3.46, a value close to the Bardeen-Cooper-Schrieffer (BCS) value of 3.53. From a detailed analysis of both the transport and thermodynamic data within the Ginsburg-Landau (GL) framework, a GL parameter of \k{appa} ~90 is obtained identifying Ta3Sb as an extreme type-II superconductor. The observation of superconductivity in an eightfold degenerate fermionic compound with topological surface states and predicted large spin Hall conductance positions Ta3Sb as an appealing platform to further explore exotic quantum states in multifold degenerate systems., Comment: 16 Pages, 3 figures

Time-domain magneto-THz spectroscopy is utilized to study the frustrated magnet averievite Cu$_{5-x}$Zn$_x$V$_2$O$_{10}$(CsCl). Pronounced THz resonances are observed in unsubstituted samples ($x=0$) when cooling below the onset of short-range magnetic correlations. The influence of external magnetic effects confirms the magnetic origin of these resonances. Increasing Zn substitution suppresses the resonances, as frustration effects dominate, reflecting the non-magnetic phases for $x> 0.25$ compounds. The temperature evolution of the THz spectra is complemented with electron spin resonance spectroscopy. This comparison allows a direct probe of the different contributions from magnetic order, frustration, and structural properties in the phase diagram of averievite. Our results illustrate the effect of magnetic interactions in THz spectra of frustrated magnets., Comment: 7 pages, 5 figures, plus supplement

We present a study of the superconducting properties of the candidate topological superconductor Ti_(3)Sb. Electrical transport measurements show zero resistance with a T_(c,onset) of ~ 5.9 K with a transition width {\Delta}T_c~ 0.6 K. The superconducting phase boundaries as derived from magneto-transport and magnetic susceptibility measurements agree well. We estimate an upper critical field Bc2(0)~4.5 T. A Ginzburg-Landau (GL) analysis yields values of the coherence length and penetration depth of {\zeta} = 6.2 nm and {\lambda} = 340 nm, respectively, and a GL parameter ~ 55, indicating extreme type-II behavior. Furthermore, we observed a step height in the specific heat ({\Delta}C_e)/({\gamma}T_c )~1.61, a value larger than the Bardeen-Cooper-Schrieffer (BCS) value of 1.43, suggesting modest coupling. Measurements of the temperature dependence of the London penetration depth via the tunnel-diode oscillator (TDO) technique down to ~ 450 mK show a full superconducting gap, consistent with a conventional s-wave gap structure., Comment: 19 pages, 6 figures

The recent reports of superconductivity in Nd(1–x)Sr(x)NiO(2)/SrTiO(3) heterostructures have reinvigorated interest in potential superconductivity of low-oxidation state nickelates. Synthesis of Ni(1+)-containing compounds is notoriously difficult. In the current work, a combined sol-gel combustion and high-pressure annealing technique was employed to prepare polycrystalline perovskite Nd(1–x)Sr(x)NiO(3) (x = 0, 0.1, and 0.2). Metal nitrates and metal acetates were used as starting materials, and the latter were found to be superior to the former in terms of safety and reactivity. The Nd(1–x)Sr(x)NiO(3) compounds were subsequently reduced to Nd(1–x)Sr(x)NiO(2) using calcium hydride in a sealed, evacuated quartz tube. To understand the synthesis pathway, the evolution from NdNiO(3) to NdNiO(2) was monitored using in situ synchrotron x-ray diffraction during the reduction process. Electrical transport properties were consistent with an insulator-metal transition occurring between x = 0 and 0.1 for Nd(1–x)Sr(x)NiO(3). Superconductivity was not observed in our bulk samples of Nd(1–x)Sr(x)NiO(2). Neutron diffraction experiments at 3 and 300 K were performed on Nd(0.9)Sr(0.1)NiO(2), in which no magnetic Bragg reflections were observed, and the results of structural Rietveld refinement are provided.

Identification, understanding, and manipulation of novel magnetic textures are essential for the discovery of new quantum materials for future spin-based electronic devices. In particular, materials that manifest a large response to external stimuli such as a magnetic field are subject to intense investigation. Here, we study the kagome-net magnet YMn

The discovery of superconductivity in a d^{9-δ} nickelate has inspired disparate theoretical perspectives regarding the essential physics of this class of materials. A key issue is the magnitude of the magnetic superexchange, which relates to whether cuprate-like high-temperature nickelate superconductivity could be realized. We address this question using Ni L-edge and O K-edge spectroscopy of the reduced d^{9-1/3} trilayer nickelates R_{4}Ni_{3}O_{8} (where R=La, Pr) and associated theoretical modeling. A magnon energy scale of ∼80 meV resulting from a nearest-neighbor magnetic exchange of J=69(4) meV is observed, proving that d^{9-δ} nickelates can host a large superexchange. This value, along with that of the Ni-O hybridization estimated from our O K-edge data, implies that trilayer nickelates represent an intermediate case between the infinite-layer nickelates and the cuprates. Layered nickelates thus provide a route to testing the relevance of superexchange to nickelate superconductivity.

A study of a dd excitation in La

Dirac and Weyl semimetals host exotic quasiparticles with unconventional transport properties, such as high magnetoresistance and carrier mobility. Recent years have witnessed a huge number of newly predicted topological semimetals from existing databases; however, experimental verification often lags behind such predictions. Common reasons are synthetic difficulties or the stability of predicted phases. Here, we report the synthesis of the type-II Dirac semimetal Ir

We studied the magnetic ordering of thin films and bulk crystals of rutile RuO_{2} using resonant x-ray scattering across the Ru L_{2} absorption edge. Combining polarization analysis and azimuthal angle dependence of the magnetic Bragg signal, we have established the presence and characteristic of collinear antiferromagnetism in RuO_{2} with T_{N}300 K. In addition to revealing a spin-ordered ground state in the simplest ruthenium oxide compound, the persistence of magnetic order even in nanometer-thick films lays the ground for potential applications of RuO_{2} in antiferromagnetic spintronics.

We report synthesis of nanowires and nanoribbons of the charge-density-wave conductor NbSe(3) through direct reaction of Nb and Se powders. The transverse dimension of the obtained nanostructures, as identified with scanning/transmission electron microscopy, ranges from 20 to 700 nm. X-ray and selected area electron diffraction analyses indicate that these nanowires and nanoribbons are single crystalline. Four-probe resistivity measurements confirm the expected charge-density-wave transitions, and furthermore, we find significant enhancement in the depinning threshold fields, which we attribute to a confinement effect.

Magnetic Compton profiles have been measured for the colossal magnetoresistance manganites La 1.2 Sr 1.8 Mn 2 O 7 and La 0.7 Sr 0.3 MnO 3 , and for magnetite Fe 3 O 4 , along various crystallographic directions, over a wide range of temperatures and magnetic fields. The experimental results are interpreted via first-principles computations for the double layer manganite, La 1.2 Sr 1.8 Mn 2 O 7 , and by using a simple model involving atomic d-orbitals and free electrons for the other two compounds. For all three materials a preference for the occupation of eg orbitals is found, particularly, for orbitals of d x 2 -y 2 symmetry. An itinerant electron contribution is adduced at all temperatures in magnetite; such a contribution also appears in La 1.2 Sr 1.8 Mn 2 O 7 , but it is present only at low temperatures in La 0.7 Sr 0.3 MnO 3 .

High-temperature superconductivity in cuprates arises from an electronic state that remains poorly understood. We report the observation of a related electronic state in a noncuprate material, strontium iridate (Sr2IrO4), in which the distinct cuprate fermiology is largely reproduced. Upon surface electron doping through in situ deposition of alkali-metal atoms, angle-resolved photoemission spectra of Sr2IrO4 display disconnected segments of zero-energy states, known as Fermi arcs, and a gap as large as 80 millielectron volts. Its evolution toward a normal metal phase with a closed Fermi surface as a function of doping and temperature parallels that in the cuprates. Our result suggests that Sr2IrO4 is a useful model system for comparison to the cuprates.

We present a detailed magnetothermal study of Pr{sub 0.7}Ca{sub 0.3}MnO{sub 3}, a perovskite manganite in which an insulator-metal transition can be driven by magnetic field, but also by pressure, visible light, x rays, or high currents. We find that the field-induced transition is associated with an enormous release of energy which accounts for its strong irreversibility. In the ferromagnetic metallic state, specific heat and magnetization measurements indicate a much smaller spin-wave stiffness than that seen in any other manganite, which we attribute to spin waves among the ferromagnetically ordered Pr moments. The coupling between the Pr and Mn spins may also provide a basis for understanding the low-temperature phase diagram of this most unusual manganite.

We report angle resolved photoemission studies of La0.66Ca0.33MnO3 and La1.2Sr1.8Mn2O7 using single crystal samples. The Mn 3p–3d resonance photoemission data of La0.66Ca0.33MnO3 show that the states at 2.5 eV binding energy have predominantly Mn 3d character, qualitatively consistent with the predictions of local spin density approximation calculations except for a 1 eV shift toward higher binding energy. Band dispersions are observed in the normal emission data. The spectra of La1.2Sr1.8Mn2O7 show well defined features and strong matrix element effects, indicating excellent surface quality.

We employed a scanning tunneling microscope to image the (001) surface topography and local density of states (LDOS) in La(2-2x)Sr(1+2x)Mn(2)O(7) (x=0.32, LSMO) single crystals below the Curie temperature (T(C)≈120 K). The LDOS maps revealed a stripelike modulation propagating along the tetragonal a axis with a wavelength of about 16 Å, which is indicative of a charge density wave (CDW). The observed CDW in the x=0.32 sample is far from the Fermi surface nesting instability as compared with the data of angle resolved photoemission spectroscopy in an x=0.40 sample. The stripe model developed previously for cuprates can explain the observed CDW in our LSMO sample, indicating that competing interactions between localized and itinerant phases are the origin of the spatial modulations present intrinsically in cuprates and manganites.

Synthesis of inorganic extended solids is a critical starting point from which real-world functional materials and their consequent technologies originate. However, unlike the rich mechanistic foundation of organic synthesis, with its underlying rules of assembly (e.g., functional groups and their reactivities), the synthesis of inorganic materials lacks an underpinning of such robust organizing principles. In the latter case, any such rules must account for the diversity of chemical species and bonding motifs inherent to inorganic materials and the potential impact of mass transport on kinetics, among other considerations. Without such assembly rules, there is less understanding, less predictive power, and ultimately less control of properties. Despite such hurdles, developing a mechanistic understanding for synthesis of inorganic extended solids would dramatically impact the range of new material discoveries and resulting new functionalities, warranting a broad call to explore what is possible. Here we discuss our recent approaches toward a mechanistic framework for the synthesis of bulk inorganic extended solids, in which either embryonic atomic correlations or fully developed phases in solutions or melts can be identified and tracked during product selection and crystallization. The approach hinges on the application of high-energy x-rays, with their penetrating power and large Q-range, to explore reaction pathways in situ. We illustrate this process using two examples: directed assembly of Zr clusters in aqueous solution and total phase awareness during crystallization from K–Cu–S melts. These examples provide a glimpse of what we see as a larger vision, in which large scale simulations, data-driven science, and in situ studies of atomic correlations combine to accelerate materials discovery and synthesis, based on the assembly of well-defined, prenucleated atomic correlations.

We used resonant inelastic x-ray scattering to reveal the nature of magnetic interactions in Sr2IrO4, a 5d transition-metal oxide with a spin-orbit entangled ground state and J(eff)=1/2 magnetic moments. The magnon dispersion in Sr2IrO4 is well-described by an antiferromagnetic Heisenberg model with an effective spin one-half on a square lattice, which renders the low-energy effective physics of Sr2IrO4 much akin to that in superconducting cuprates. This point is further supported by the observation of exciton modes in Sr2IrO4, whose dispersion is strongly renormalized by magnons, which can be understood by analogy to hole propagation in the background of antiferromagnetically ordered spins in the cuprates.

We report an inelastic neutron scattering study of acoustic phonons in the charge and orbitally ordered bilayer manganite LaSr(2)Mn(2)O(7). For excitation energies less than 15 meV, we observe an abrupt increase (decrease) of the phonon energies (linewidths) of a transverse acoustic phonon branch at q = (h, h, 0), h ≤ 0.3, upon entering the low temperature charge and orbital ordered state (T(COO) = 225 K). This indicates a reduced electron-phonon coupling due to a decrease of electronic states at the Fermi level leading to a partial removal of the Fermi surface below T(COO) and provides direct experimental evidence for a link between electron-phonon coupling and charge order in manganites.

The evolution of the short-range structural signature of the Ir4+ dimer state in CuIr2S4 thiospinel has been studied across the metal-insulator phase transitions as the metallic state is induced by temperature, Cr doping, and x-ray fluence. An atomic pair distribution function (PDF) approach reveals that there are no local dimers that survive into the metallic phase when this is invoked by temperature and doping. The PDF shows Ir4+ dimers when they exist, regardless of whether or not they are long-range ordered. At 100 K, exposure to a 98 keV x-ray beam melts the long-range dimer order within a few seconds, though the local dimers remain intact. This shows that the metallic state accessed on warming and doping is qualitatively different from the state obtained under x-ray irradiation.

We have studied the frustrated system YBaCo4O7.0 generally described as an alternating stacking of kagome and triangular layers of magnetic ions on a trigonal lattice, by single-crystal neutron diffraction experiments above the Néel ordering transition. Experimental data reveal pronounced magnetic diffuse scattering, which is successfully modeled by direct Monte Carlo simulations. Long-range magnetic correlations are found along the c axis, due to the presence of corner-sharing bipyramids, creating quasi-one-dimensional order at finite temperature. In contrast, in the kagome layers (ab plane), the spin-spin correlation function, displaying a short-range 120 degrees configuration, decays rapidly as typically found in spin liquids. YBaCo4O7 experimentally realizes a new class of two-dimensional frustrated systems where the strong out-of-plane coupling does not lift the in-plane degeneracy, but instead acts as an external "field."

We report the magnetic and electrical characteristics of polycrystalline FeTiO_{3} synthesized at high pressure that is isostructural with acentric LiNbO_{3} (LBO). Piezoresponse force microscopy, optical second harmonic generation, and magnetometry demonstrate ferroelectricity at and below room temperature and weak ferromagnetism below approximately 120 K. These results validate symmetry-based criteria and first-principles calculations of the coexistence of ferroelectricity and weak ferromagnetism in a series of transition metal titanates crystallizing in the LBO structure.

Low temperature Mn K-edge x-ray magnetic circular dichroism and x-ray diffraction measurements were carried out to investigate the stability of the ferromagnetic ground state in manganite La0.75Ca0.25MnO3 under nearly uniform compression using diamond anvil cells. The magnetic dichroism signal gradually decreases with pressure and disappears at 23 GPa, and meanwhile a uniaxial compression of MnO6 octahedra along the b axis is observed to continuously increase with pressure and become anomalously large at 23.5 GPa. These changes are attributed to a ferromagnetic-antiferromagnetic transition that is associated with orbital ordering at high pressure.

The combined local structure techniques, extended x-ray absorption fine structure and neutron pair distribution function analysis, have been used for temperatures 4or =Tor =330 K to rule out a large Jahn-Teller (JT) distortion of the Co-O bond in La1-xSrxCoO3 for a significant fraction of Co sites (xor =0.35), indicating few, if any, JT-active, singly occupied e_{g} Co sites exist.

The detailed evolution of the magnitude of the local Jahn-Teller (JT) distortion in La(1-x)Ca(x)MnO3 is obtained across the phase diagram for 0or =xor =0.5 from high-quality neutron diffraction data using the atomic pair distribution function method. A local JT distortion is observed in the insulating phase for all Ca concentrations studied. However, in contrast with earlier local structure studies, its magnitude is not constant, but decreases continuously with increasing Ca content. This observation is at odds with a simple small-polaron picture for the insulating state.

Contrary to conventional wisdom, our purified La 2-2x Sr 1+2x Mn2O7 crystals exhibit CE-type orbital and charge order as the low-temperature ground state for a hole doping level h=0.5. For small deviations from h=0.5, the high-temperature CE phase is replaced at low temperatures by an A-type antiferromagnet without coexistence. Larger deviations result in a lack of CE order at any temperature. Thus, small inhomogeneities in cation or oxygen composition could explain why others commonly see this reentrance with coexistence.

Using angle-resolved photoemission, we have observed sharp quasiparticlelike peaks in the prototypical layered manganite La(2-2x)Sr(1+2x)Mn(2)O(7) (x=0.36,0.38). We focus on the (pi,0) regions of k space and study their electronic scattering rates and dispersion kinks, uncovering bilayer-split bands, the critical energy scales, momentum scales, and strengths of the interactions that renormalize the electrons. To identify these bosons, we measured phonon dispersions in the energy range of the kink by inelastic neutron scattering, finding a good match in both energy and momentum to the oxygen bond-stretching phonons.