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Register a new userLithium Ruthenates: Controlling Dimensionality and Topology of Magnetic-Ion Arrangements
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In order to control the dimensionality and the topology of the arrangement of magnetic Ru ions, NaCl-type lithium ruthenates have been investigated. Three types of lithium ruthenates, Li$_{3}$RuO$_{4}$, Li$_{2}$RuO$_{3}$, and cubic-Li$_{x}$RuO$_{1+x}$, were synthesized using a hydrothermal method. All of them have NaCl-type structure, but the arrangements of the cations, Li$^{+}$ and Ru$^{5+}$ (or Ru$^{4+}$), differ from each other. Li$_{3}$RuO$_{4}$ with one-dimensional zigzag chains of Ru ions undergoes an antiferromagnetic transition at 66 K and exhibits an irreversibile magnetism below 32 K, where the zero-field-cooled susceptibility differs from the field-cooled susceptibility. Li$_{2}$RuO$_{3}$ with a two-dimensional honeycomb network of Ru ions demonstrates a paramagnetism almost independent of temperature. A novel ruthenate cubic-Li$_{x}$RuO$_{1+x}$, in which Ru and Li randomly occupy the cation sites of NaCl lattice, undergoes a spin-glass transition at 10 K.
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The effects of competing magnetic interactions in stabilizing different spin configurations are drawing a renewed attention in order to both unveil emerging topological spin textures and to highlight microscopic mechanisms leading to their stabilization. The possible key role of the two-site exchange anisotropy in selecting specific helicity and vorticity of skyrmionic lattices has only recently been proposed. In this work we explore the phase diagram of a frustrated localized magnet on a two-dimensional centrosymmetric triangular lattice, focusing on the interplay between the two-ion anisotropy (TIA) and the single-ion anisotropy (SIA). The effects of an external magnetic field applied perpendicularly to the magnetic layer are also investigated. By means of Monte Carlo simulations, we find a profusion of different spin configurations, going from trivial to high-order Q skyrmionic and meronic lattices. In closer detail, we find that a dominant role is played by the two-ion over the single-ion anisotropy in determining the planar spin texture, whereas the strength and sign of SIA, together with the magnitude of the magnetic field, tune the perpendicular spin components, mostly affecting the polarity (and, in turn, the topology) of the spin-texture. Our analysis confirms the crucial role of anisotropic symmetric exchange in systems with dominant short-range interactions, at the same time predicting a rich variety of complex magnetic textures that may arise from a fine tuning of competing anisotropic mechanisms.
Neutron diffraction and magnetic susceptibility studies show that orthorhombic single-crystals of topological semimetals ${rm Sr(Mn_{0.9}Cu_{0.1})Sb_2}$ and ${rm Sr(Mn_{0.9}Zn_{0.1})Sb_2}$ undergo three dimensional C-type antiferromagnetic (AFM) ordering of the Mn$^{2+}$ moments at $T_N = 200pm10$ and $210pm12$ K, respectively, significantly lower than that of the parent SrMnSb$_2$ with $T_N=297 pm 3$ K. Magnetization versus applied magnetic field (perpendicular to MnSb planes) below $T_N$ exhibits slightly modified de Haas van Alphen oscillations for the Zn-doped crystal as compared to that of the parent compound. By contrast, the Cu-doped system does not show de Haas van Alphen magnetic oscillations, suggesting that either Cu substitution for Mn changes the electronic structure of the parent compound substantially, or that the Cu sites are strong scatterers of carriers that significantly shorten their mean free path thus diminishing the oscillations. Density functional theory (DFT) calculations including spin-orbit coupling predict the C-type AFM state for the parent, Cu-, and Zn-doped systems and identify the $a$-axis (i.e., perpendicular to the Mn layer) as the easy magnetization direction in the parent and 12.5% of Cu or Zn substitutions. In contrast, 25% of Cu content changes the easy magnetization to the $b$-axis (i.e., within the Mn layer). We find that the incorporation of Cu and Zn in SrMnSb$_2$ tunes electronic bands near the Fermi level resulting in different band topology and semi-metallicity. The parent and Zn-doped systems have coexistence of electron and hole pockets with opened Dirac cone around the Y-point whereas the Cu-doped system has dominant hole pockets around the Fermi level with a distorted Dirac cone. The tunable electronic structure may point out possibilities of rationalizing the experimentally observed de Haas van Alphen magnetic oscillations.
A thick electrode with high areal capacity has been developed as a strategy for high-energy-density lithium-ion batteries, but thick electrodes have difficulties in manufacturing and limitations in ion transport. Here, we reported a new manufacturing approach for ultra-thick electrode with aligned structure, called structure electrode additive manufacturing or SEAM, which aligns active materials to the through-thicknesses direction of electrodes using shear flow and a designed printing path. The ultra-thick electrodes with high loading of active materials, low tortuous structure, and good structure stability resulting from a simple and scalable SEAM lead to rapid ion transport and fast electrolyte infusion, delivering a higher areal capacity than slurry-casted thick electrodes. SEAM shows strengths in design flexibility and scalability, which allows the production of practical high energy/power density structure electrodes.
Li-ion rechargeable batteries have enabled the wireless revolution transforming global communication. Future challenges, however, demands distributed energy supply at a level that is not feasible with the current energy-storage technology. New materials, capable of providing higher energy density are needed. Here we report a new class of lithium-ion batteries based on a graphene ink anode and a lithium iron phosphate cathode. By carefully balancing the cell composition and suppressing the initial irreversible capacity of the anode, we demonstrate an optimal battery performance in terms of specific capacity, i.e. 165 mAhg-1, estimated energy density of about 190 Whkg-1 and life, with a stable operation for over 80 charge-discharge cycles. We link these unique properties to the graphene nanoflake anode displaying crystalline order and high uptake of lithium at the edges, as well as to its structural and morphological optimization in relation to the overall battery composition. Our approach, compatible with any printing technologies, is cheap and scalable and opens up new opportunities for the development of high-capacity Li-ion batteries.
Defects intentionally introduced into magnetic materials often have a profound effect on the physical properties. Specifically tailored neutron spectroscopic experiments can provide detailed information on both the local exchange interactions and the local distances between the magnetic atoms around the defects. This is demonstrated for manganese dimer excitations observed for the magnetically diluted three- and two-dimensional compounds KMn(x)Zn(1-x)F(3) and K(2)Mn(x)Zn(1-x)F(4), respectively. The resulting local exchange interactions deviate up to 10% from the average, and the local Mn-Mn distances are found to vary stepwise with increasing internal pressure due to the Mn/Zn substitution. Our analysis qualitatively supports the theoretically predicted decay of atomic displacements according to 1/r**2, 1/r, and constant (for three-, two-, and one-dimensional compounds, respectively) where r denotes the distance of the displaced atoms from the defect.
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