Julia Y. Chan

Realization of a three-dimensional spin–anisotropic harmonic honeycomb iridate

The physics of Mott insulators underlies diverse phenomena ranging from high temperature superconductivity to exotic magnetism. Although both the electron spin and the structure of the local orbitals play a key role in this physics, in most systems these are connected only indirectly — via the Pauli exclusion principle and the Coulomb interaction. Iridium-based oxides (iridates) open a further dimension to this problem by introducing strong spin-orbit interactions, such that the Mott physics has a strong orbital character. In the layered honeycomb iridates this is thought to generate highly spin-anisotropic interactions, coupling the spin orientation to a given spatial direction of exchange and leading to strongly frustrated magnetism. The potential for new physics emerging from such interactions has driven much scientific excitement, most recently in the search for a new quantum spin liquid, first discussed by Kitaev [1]. Here we report a new iridate structure that has the same local connectivity as the layered honeycomb, but in a three-dimensional framework. The temperature dependence of the magnetic susceptibility exhibits a striking reordering of the magnetic anisotropy, giving evidence for highly spin-anisotropic exchange interactions. Furthermore, the basic structural units of this material suggest the possibility of a new family of structures, the ‘harmonic honeycomb’ iridates. This compound thus provides a unique and exciting glimpse into the physics of a new class of strongly spin-orbit coupled Mott insulators. ∗ These authors contributed equally to this work.

Probing the Lower Limit of Lattice Thermal Conductivity in an Ordered Extended Solid: Gd117Co56Sn112, a Phonon Glass–Electron Crystal System

The discovery of novel materials with low thermal conductivity is paramount to improving the efficiency of thermoelectric devices. As lattice thermal conductivity is inversely linked to unit cell complexity, we set out to synthesize a highly complex crystalline material with glasslike thermal conductivity. Here we present the structure, transport properties, heat capacity, and magnetization of single-crystal Gd(117)Co(56)Sn(112), a complex material with a primitive unit cell volume of ~6858 Å(3) and ~285 atoms per primitive unit cell (1140 atoms per face-centered cubic unit cell). The room temperature lattice thermal conductivity of this material is κ(L) = 0.28 W/(m·K) and represents one of the lowest ever reported for a nonglassy or nonionically conducting bulk solid. Furthermore, this material exhibits low resistivity at room temperature, and thus represents a true physical system that approaches the ideal phonon glass-electron crystal.

Nanoimprinted Perovskite Nanograting Photodetector with Improved Efficiency

Recently, organolead halide-based perovskites have emerged as promising materials for optoelectronic applications, particularly for photovoltaics, photodetectors, and lasing, with low cost and high performance. Meanwhile, nanoscale photodetectors have attracted tremendous attention toward realizing miniaturized optoelectronic systems, as they offer high sensitivity, ultrafast response, and the capability to detect beyond the diffraction limit. Here we report high-performance nanoscale-patterned perovskite photodetectors implemented by nanoimprint lithography (NIL). The spin-coated lead methylammonium triiodide perovskite shows improved crystallinity and optical properties after NIL. The nanoimprinted metal-semiconductor-metal photodetectors demonstrate significantly improved performance compared to the nonimprinted conventional thin-film devices. The effects of NIL pattern geometries on the optoelectronic characteristics were studied, and the nanograting pattern based photodetectors demonstrated the best performance, showing approximately 35 times improvement on responsivity and 7 times improvement on on/off ratio compared with the nonimprinted devices. The high performance of NIL-nanograting photodetectors likely results from high crystallinity and favored nanostructure morphology, which contribute to higher mobility, longer diffusion length, and better photon absorption. Our results have demonstrated that the NIL is a cost-effective method to fabricate high-performance perovskite nanoscale optoelectronic devices, which may be suitable for manufacturing of high-density perovskite nanophotodetector arrays and to provide integration with state-of-the-art electronic circuits.

Electrodeposition of FeCoNiCu/Cu Compositionally Modulated Multilayers

The electrodeposition of the FeCoNiCu quaternary system onto a rotating disk electrode was explored in order to prepare compositionally modulated multilayers. Multilayers having a different layer thickness were electrodeposited by a pulse current method and the structure was determined with transmission electron microscopy and X-ray diffraction. When the multilayer alloy thickness was larger than 10 nm, the deposit grain size was found to be a function of the Co-rich layer thickness. Below an alloy thickness of 10 nm, the Cu layer size was correlated with a preferred deposit orientation. Giant magnetoresistance was also observed for this electrodeposited quaternary system for the first time.

Phase diagram and magnetocaloric effects in aluminum doped MnNiGe alloys

The magnetocaloric and thermomagnetic properties of the MnNiGe1−xAlx system have been studied by temperature-dependent x-ray diffraction, differential scanning calorimetry (DSC), and magnetization measurements. The partial substitution of Al for Ge in MnNiGe1−xAlx results in a first order magnetostructural transition (MST) from a hexagonal ferromagnetic to an orthorhombic antiferromagnetic phase at 186 K (for x = 0.09). A large magnetic entropy change of ΔSM = −17.6 J/kg K for ΔH = 5 T was observed in the vicinity of TM = 186 K for x = 0.09. The value is comparable to those of giant magnetocaloric materials such as Gd5Si2Ge2, MnFeP0.45As0.55, and Ni50Mn37Sn13. The values of the latent heat (L = 6.6 J/g) and corresponding total entropy changes (ΔST = 35 J/kg K) have been evaluated for the MST using DSC measurements. Large negative values of ΔSM of −5.8 and −4.8 J/kg K for ΔH = 5 T in the vicinity of TC were observed for x = 0.09 and 0.085, respectively. A concentration-dependent phase diagram of transition...

Discovery of the Griffiths phase in the itinerant magnetic semiconductor Fe1-xCoxS2.

Critical points that can be suppressed to zero temperature are interesting because quantum fluctuations have been shown to dramatically alter electron gas properties. Here, the metal formed by Co doping the paramagnetic insulator FeS2, Fe1-xCoxS2 is demonstrated to order ferromagnetically at x > xc = 0.01+/-0.005, where we observe unusual transport, magnetic, and thermodynamic properties. We show that this magnetic semiconductor undergoes a percolative magnetic transition with distinct similarities to the Griffiths phase, including singular behavior at xc and zero temperature.

Synthesis, structure, and magnetism of a new heavy-fermion antiferromagnet, CePdGa6

Abstract A new compound, CePdGa 6 , and its isostructural analog, LaPdGa 6 have been synthesized by flux growth and characterized by single-crystal X-ray diffraction. The compounds adopt a tetragonal structure with P 4/ mmm space group, Z =1. The lattice parameters for CePdGa 6 are a=b=4.350(3) A and c=7.922(6) A and a=b=4.3760(3) A and c=7.9230(5) A for LaPdGa 6 . Magnetic and thermal measurement have revealed that CePdGa 6 is a heavy-fermion with the specific heat coefficient γ∼300 mJ / mol K 2 and Ce f moments order antiferromagnetically along c -axis at T N =10 K . Reconfiguration of spin occurs at 5 K to induce a ferromagnetic component only in the a–b plane. This strong anisotropy in the magnetism might be related to its unique layered structure.

High resolution three-dimensional visualization and characterization of coronary atherosclerosis in vitro by synchrotron radiation x-ray microtomography and highly localized x-ray diffraction

Human atherosclerotic plaques in both native and bypass arteries have been visualized using microtomography to provide additional information on the nature of coronary artery disease. Plaques contained within arteries removed from three white males aged 51, 55 and 70 are imaged in three-dimensions with monochromatic synchrotron x-ray radiation. Fields of view are 658 x 658 x 517 voxels. with cubic voxels ranging from 12 to 13 microm on a side. X-ray energies range from 11 to 15 keV (bandpass approximately 10 eV). At lower energies, high local absorption tends to generate reconstruction artefacts, while at higher energies the arterial wall is scarcely visible. At all energies, calcifications are clearly visible and differences are observed between plaques in native arteries (lifetime accumulations) versus bypass arteries (plaques developing in the interval between the heart bypass operation and the autopsy). In order to characterize coronary calcification, a microfocused, 50 microm2, 25 keV x-ray beam was used to acquire powder diffraction data from selected calcifications. Also, large calcifications were removed from the native arteries and imaged with 25 keV x-ray energy. Calcifications are composed of hydroxyapatite crystallites and an amorphous phase. In summary, native calcifications are larger and have a higher fraction of hydroxyapatite than calcifications from the bypass arteries.

Successive phase transitions and phase diagrams for the quasi-two-dimensional easy-axis triangular antiferromagnet Rb4Mn(MoO4)3

Using magnetic, thermal and neutron measurements we show that Rb4Mn(MoO4)3 is a quasi-2D triangular Heisenberg antiferromagnet with easy-axis anisotropy and successive transitions bracketing an intermediate collinear phase. An accurate quantitative account of the phase diagram is achieved through Monte Carlo simulation of a spin Hamiltonian with easy-axis anisotropy D=0.22J.

Crystal Growth, Transport, and the Structural and Magnetic Properties of Ln4FeGa12 with Ln = Y, Tb, Dy, Ho, and Er

Ln(4)FeGa(12), where Ln is Y, Tb, Dy, Ho, and Er, prepared by flux growth, crystallize with the cubic Y(4)PdGa(12) structure with the Im3m space group and with a = 8.5650(4), 8.5610(4), 8.5350(3), 8.5080(3), and 8.4760(3) A, respectively. The crystal structure consists of an iron-gallium octahedra and face-sharing rare-earth cuboctahedra of the Au(3)Cu type. Er(4)Fe(0.67)Ga(12) is iron-deficient, leading to a distortion of the octahedral and cuboctahedral environments due to the splitting of the Ga2 site into Ga2 and Ga3 sites. Further, interstitial octahedral sites that are unoccupied in Ln(4)FeGa(12) (Ln = Y, Tb, Dy, and Ho) are partially occupied by Fe2. Y(4)FeGa(12) exhibits weak itinerant ferromagnetism below 36 K. In contrast, Tb(4)FeGa(12), Dy(4)FeGa(12), Ho(4)FeGa(12), and Er(4)Fe(0.67)Ga(12) order antiferromagnetically with maxima in the molar magnetic susceptibilities at 26, 18.5, 9, and 6 K. All of the compounds exhibit metallic electric resistivity, and their iron-57 Mossbauer spectra, obtained between 4.2 and 295 K, exhibit a single-line absorption with a 4.2 K isomer shift of ca. 0.50 mm/s, a shift that is characteristic of iron in an iron-gallium intermetallic compound. A small but significant broadening in the spectral absorption line width is observed for Y(4)FeGa(12) below 40 K and results from the small hyperfine field arising from its spin-polarized itinerant electrons.