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A. Senyshyn

Publications and source records attributed to A. Senyshyn.

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Magnetic properties of the noncentrosymmetric tetragonal antiferromagnet EuPtSi$_{3}$

We report a comprehensive study of single crystals of the noncentrosymmetric rare-earth compound EuPtSi$_{3}$ grown by the optical floating-zone technique. Measurements of the magnetization, ac susceptibility, and specific heat consistently establish antiferromagnetic order of localized Eu$^{2+}$ moments below the Néel temperature $T_{\mathrm{N}} = 17~\mathrm{K}$, followed by a second magnetic transition at $T_{\mathrm{N1}} = 16~\mathrm{K}$. For a magnetic field along the easy $[001]$ axis, the magnetic phase diagram is composed of these two phases. For fields applied in the magnetically hard basal plane, two additional phases emerge under magnetic field, where the in-plane anisotropy is weak with $[100]$ being the hardest axis. At the phase transitions, the magnetic properties exhibit hysteresis and discrepancies between differential and ac susceptibility, suggesting slow reorientation processes of mesoscale magnetic textures. Consistently, powder and single-crystal neutron diffraction in zero field identify magnetic textures that are modulated on a length scale of the order of $100~\textrm{Å}$, most likely in the form of Néel-type antiferromagnetic cycloids.

cond-mat.str-el

Structural and magnetic properties of the new quantum magnet BaCuTe$_2$O$_6$

We investigate the structural and magnetic properties of the new quantum magnet BaCuTe$_2$O$_6$. This compound is synthesized for the first time in powder and single crystal form. Synchrotron X-ray and neutron diffraction reveal a cubic crystal structure (P4$_1$32) where the magnetic Cu$^{2+}$ ions form a complex network. Physical properties measurements suggest the presence of antiferromagnetic interactions with a Curie-Weiss temperature of -33K, while long-range magnetic order occurs at the much lower temperature of ~6.3K. The magnetic structure, solved using neutron diffraction, reveals antiferromagnetic order along chains parallel to the a, b and c crystal axes. This is consistent with the magnetic excitations which resemble the multispinon continuum typical of the spin-1/2 Heisenberg antiferromagnetic chain. A consistent intrachain interaction value of ~34K is achieved from the various techniques. Finally the magnetic structure provides evidence that the chains are coupled together in a non-colinear arrangement by a much weaker antiferromagnetic, frustrated hyperkagome interaction.

cond-mat.str-el

MnSnTeO6: a Chiral Antiferromagnet Prepared by a Two-Step Topotactic Transformation

MnSnTeO6, a new chiral antiferromagnet, was prepared both by topotactic transformation of the metastable rosiaite-type polymorph and by direct synthesis from coprecipitated hydroxides. Its structure, static and dynamic magnetic properties were studied comprehensively both experimentally (through X-ray and neutron powder diffraction, magnetization, specific heat, dielectric permittivity and ESR techniques) and theoretically (by means of ab initio density functional theory (DFT) calculations within the spin-polarized generalized gradient approximation). MnSnTeO6 is isostructural with MnSb2O6 (space group P321) and does not show any structural transition between 3 and 300 K. The magnetic susceptibility and specific heat exhibit an antiferromagnetic ordering at TN=9.8 K, which is confirmed by low-temperature neutron data. At the same time, the thermodynamic parameters demonstrate an additional anomaly on the temperature dependences of magnetic susceptibility chi(T), specific heat Cp(T) and dielectric permittivity epsilon(T) at T*=4.9 K, which is characterized by significant temperature hysteresis. Clear enhancement of the dielectric permittivity at T* is most likely to reflect the coupling of dielectric and magnetic subsystems leading to development of electric polarization. It was established that the ground state of MnSnTeO6 is stabilized by seven exchange parameters, and neutron diffraction revealed incommensurate magnetic structure with propagation vector k= (0, 0, 0.183) analogous to that of MnSb2O6. Ab initio DFT calculations demonstrate that the strongest exchange coupling occurs between planes along diagonals. All exchange parameters are antiferromagnetic and reveal moderate frustration.

cond-mat.str-el

Origin of Ferroelectricity in Orthorhombic LuFeO$_3$

We demonstrate that small but finite ferroelectric polarization ($\sim$0.01 $μ$C/cm$^2$) emerges in orthorhombic LuFeO$_3$ ($Pnma$) at $T_N$ ($\sim$600 K) because of commensurate (k = 0) and collinear magnetic structure. The synchrotron x-ray and neutron diffraction data suggest that the polarization could originate from enhanced bond covalency together with subtle contribution from lattice. The theoretical calculations indicate enhancement of bond covalency as well as the possibility of structural transition to the polar $Pna2_1$ phase below $T_N$. The $Pna2_1$ phase, in fact, is found to be energetically favorable below $T_N$ in orthorhombic LuFeO$_3$ ($albeit$ with very small energy difference) than in isostructural and nonferroelectric LaFeO$_3$ or NdFeO$_3$. Application of electric field induces finite piezostriction in LuFeO$_3$ via electrostriction resulting in clear domain contrast images in piezoresponse force microscopy.

cond-mat.str-el

Superionic diffusion through frustrated energy landscape

Solid-state materials with high ionic conduction are necessary to many technologies including all-solid-state Li-ion batteries. Understanding how crystal structure dictates ionic diffusion is at the root of the development of fast ionic conductors. Here, we show that LiTi2(PS4)3 exhibits a Li-ion diffusion coefficient about an order of magnitude higher than current state-of-the-art lithium superionic conductors. We rationalize this observation by the unusual crystal structure of LiTi2(PS4)3 which offers no regular tetrahedral or octahedral sites for lithium to favorably occupy. This creates a smooth, frustrated energy landscape resembling more the energy landscapes present in liquids than in typical solids. This frustrated energy landscape leads to a high diffusion coefficient combining low activation energy with a high pre-factor.

cond-mat.mtrl-sci

Putative spin-nematic phase in BaCdVO(PO$_{4}$)$_{2}$

We report neutron scattering and AC magnetic susceptibility measurements of the 2D spin-1/2 frustrated magnet BaCdVO(PO$_{4}$)$_{2}$. At temperatures well below $T_{\sf N}\approx 1K$, we show that only 34 % of the spin moment orders in an up-up-down-down strip structure. Dominant magnetic diffuse scattering and comparison to published $μ$sr measurements indicates that the remaining 66 % is fluctuating. This demonstrates the presence of strong frustration, associated with competing ferromagnetic and antiferromagnetic interactions, and points to a subtle ordering mechanism driven by magnon interactions. On applying magnetic field, we find that at $T=0.1$ K the magnetic order vanishes at 3.8 T, whereas magnetic saturation is reached only above 4.5 T. We argue that the putative high-field phase is a realization of the long-sought bond-spin-nematic state.

cond-mat.str-el

Canted antiferromagnetism in phase-pure CuMnSb

We report the low-temperature properties of phase-pure single crystals of the half-Heusler compound CuMnSb grown by means of optical float-zoning. The magnetization, specific heat, electrical resistivity, and Hall effect of our single crystals exhibit an antiferromagnetic transition at $T_{\mathrm{N}} = 55~\mathrm{K}$ and a second anomaly at a temperature $T^{*} \approx 34~\mathrm{K}$. Powder and single-crystal neutron diffraction establish an ordered magnetic moment of $(3.9\pm0.1)~μ_{\mathrm{B}}/\mathrm{f.u.}$, consistent with the effective moment inferred from the Curie-Weiss dependence of the susceptibility. Below $T_{\mathrm{N}}$, the Mn sublattice displays commensurate type-II antiferromagnetic order with propagation vectors and magnetic moments along $\langle111\rangle$ (magnetic space group $R[I]3c$). Surprisingly, below $T^{*}$, the moments tilt away from $\langle111\rangle$ by a finite angle $δ\approx 11^{\circ}$, forming a canted antiferromagnetic structure without uniform magnetization consistent with magnetic space group $C[B]c$. Our results establish that type-II antiferromagnetism is not the zero-temperature magnetic ground state of CuMnSb as may be expected of the face-centered cubic Mn sublattice.

cond-mat.str-el

Persistent low-temperature spin dynamics in the mixed-valence iridate Ba$_{3}$InIr$_{2}$O$_{9}$

Using thermodynamic measurements, neutron diffraction, nuclear magnetic resonance, and muon spin relaxation, we establish putative quantum spin-liquid behavior in Ba$_3$InIr$_2$O$_9$, where unpaired electrons are localized on mixed-valence Ir$_2$O$_9$ dimers with Ir$^{4.5+}$ ions. Despite the antiferromagnetic Curie-Weiss temperature on the order of 10 K, neither long-range magnetic order nor spin freezing are observed down to at least 20 mK, such that spins are short-range correlated and dynamic over nearly three decades in temperature. Quadratic power-law behavior of both the spin-lattice relaxation rate and specific heat indicates the gapless nature of the ground state. We envisage that this exotic behavior may be related to an unprecedented combination of the triangular and buckled honeycomb geometries of nearest-neighbor exchange couplings in the mixed-valence setting.

cond-mat.str-el

Room temperature tetragonal noncollinear antiferromagnet Pt$_2$MnGa

Here we present the tetragonal stoichiometric Heusler compound Pt$_2$MnGa with the noncollinear AFM order stable up to 350 K. It is resolved by the neutron diffraction as a helical spiral propagating along the tetragonal axis. Ab-initio calculations suggest a pure exchange origin of the spiral and explain its helical character being stabilized by a large basal plane magnetocrystalline anisotropy (MCA). Together with the inversion-symmetric crystal structure, this provides a bi-stability of a spiral with respect to the right- and left-handed magnetic helices. Despite the large MCA, the long period of a helix might greatly facilitate the switch of the helicity by the precessional reorientation, suggesting Pt$_2$MnGa as a potential candidate for the vector-helicity based non-volatile magnetic memory.

cond-mat.mtrl-sci

Single crystal growth of CeTAl$_3$ (T = Cu, Ag, Au, Pd and Pt)

We report single crystal growth of the series of CeTAl$_3$ compounds with T = Cu, Ag, Au, Pd and Pt by means of optical float zoning. High crystalline quality was confirmed in a thorough characterization process. With the exception of CeAgAl$_3$, all compounds crystallize in the non-centrosymmetric tetragonal BaNiSn$_{3}$ structure (space group: I4mm, No. 107), whereas CeAgAl$_3$ adopts the related orthorhombic PbSbO$_2$Cl structure (Cmcm, No. 63). An attempt to grow CeNiAl$_3$ resulted in the composition CeNi$_2$Al$_5$. Low temperature resistivity measurements down to $\sim$0.1K did not reveal evidence suggestive of magnetic order in CePtAl$_3$ and CePdAl$_3$. In contrast, CeAuAl$_3$, CeCuAl$_3$ and CeAgAl$_3$ display signatures of magnetic transitions at 1.3K, 2.1K and 3.2K, respectively. This is consistent with previous reports of antiferromagnetic order in CeAuAl$_3$, and CeCuAl$_3$ as well as ferromagnetism in CeAgAl$_3$, respectively.

cond-mat.str-el

Homogeneity of lithium distribution in cylinder-type Li-ion batteries

Spatially-resolved neutron powder diffraction with gauge volume 2x2x20 mm3 has been applied to probe the lithium concentration in the graphite anode of different Li-ion cells of 18650-type in situ in charged state. Structural studies performed in combination with electrochemical measurements and X-ray computed tomography under real cell operating conditions unambiguously revealed non-homogeneity of lithium distribution in the graphite anode. Deviations from a homogeneous behaviour have been found in both radial and axial directions of 18650-type cells and were discussed in the frame of cell geometry and electrical connection of electrodes, which might play a crucial role in the homogeneity of the lithium distribution in the active materials within each electrode.

cond-mat.mtrl-sci

New Diluted Ferromagnetic Semiconductor isostructural to 122 type iron pnictide superconductor with TC up to 180 K

Diluted magnetic semiconductors (DMS) have received much attention due to its potential applications to spintronics devices. A prototypical system (Ga,Mn)As has been widely studied since 1990s. The simultaneous spin and charge doping via hetero-valence (Ga3+,Mn2+) substitution, however, resulted in severely limited solubility without availability of bulk specimens. Previously we synthesized a new diluted ferromagnetic semiconductor of bulk Li(Zn,Mn)As with Tc up to 50K, where isovalent (Zn,Mn) spin doping was separated from charge control via Li concentrations. Here we report the synthesis of a new diluted ferromagnetic semiconductor (Ba1-xKx)(Zn1-yMny)2As2, isostructural to iron 122 system, where holes are doped via (Ba2+, K1+), while spins via (Zn2+,Mn2+) substitutions. Bulk samples with x=0.1-0.3 and y=0.05-0.15 exhibit ferromagnetic order with TC up to 180K, comparable to that of record high Tc for Ga(MnAs), significantly enhanced than Li(Zn,Mn)As. Moreover the (Ba,K)(Zn,Mn)2As2 shares the same 122 crystal structure with semiconducting BaZn2As2, antiferromagnetic BaMn2As2, and superconducting (Ba,K)Fe2As2, which makes them promising to the development of multilayer functional devices.

cond-mat.mtrl-sci

Magnetostrictive Neel ordering of the spin-5/2 ladder compound BaMn2O3: distortion-induced lifting of geometrical frustration

The crystal structure and the magnetism of BaMn$_2$O$_3$ have been studied by thermodynamic and by diffraction techniques using large single crystals and powders. BaMn$_2$O$_3$ is a realization of a $S = 5/2$ spin ladder as the magnetic interaction is dominant along 180$^\circ$ Mn-O-Mn bonds forming the legs and the rungs of a ladder. The temperature dependence of the magnetic susceptibility exhibits well-defined maxima for all directions proving the low-dimensional magnetic character in BaMn$_2$O$_3$. The susceptibility and powder neutron diffraction data, however, show that BaMn$_2$O$_3$ exhibits a transition to antiferromagnetic order at 184 K, in spite of a full frustration of the nearest-neighbor inter-ladder coupling in the orthorhombic high-temperature phase. This frustration is lifted by a remarkably strong monoclinic distortion which accompanies the magnetic transition.

cond-mat.str-el

Magnetic structure and orbital ordering in KCrF3 perovskite

KCrF3 represents another prototypical orbital-ordered perovskite, where Cr2+ possesses the same electronic configuration of 3d4 as that of strongly Jahn-Teller distorted Mn3+ in many CMR manganites. The crystal and magnetic structures of KCrF3 compound are investigated by using polarized and unpolarized neutron powder diffraction methods. The results show that the KCrF3 compound crystallizes in tetragonal structure at room temperature and undergoes a monoclinic distortion with the decrease in temperature. The distortion of the crystal structure indicates the presence of cooperative Jahn-Teller distortion which is driven by orbital ordering. With decreasing temperature, four magnetic phase transitions are observed at 79.5, 45.8, 9.5, and 3.2 K, which suggests a rich magnetic phase diagram. Below T_N = 79.5 K, the Cr2+ moment orders in an incommensurate antiferromagnetic arrangement, which can be defined by the magnetic propagation vector (1/2$\pm\,$$δ\,$, 1/2$\pm\,$$δ\,$, 0). The incommensurate-commensurate magnetic transition occurs at 45.8 K and the magnetic propagation vector locks into (1/2, 1/2, 0) with the Cr moment of 3.34(5) $μ_B \,$ aligned ferromagnetically in (220) plane, but antiferromagnetically along [110] direction. Below 9.5 K, the canted antiferromagnetic ordering and weak ferromagnetism arise from the collinear antiferromagnetic structure, while the Dzyaloshinskii-Moriya interaction and tilted character of the single-ion anisotropy might give rise to the complex magnetic behaviors below 9.5 K.

cond-mat.str-el

CaCrO3: an anomalous antiferromagnetic metallic oxide

Combining infrared reflectivity, transport, susceptibility and several diffraction techniques, we find compelling evidence that CaCrO3 is a rare case of a metallic and antiferromagnetic transition-metal oxide with a three-dimensional electronic structure. LSDA calculations correctly describe the metallic behavior as well as the anisotropic magnetic ordering pattern of C type: The high Cr valence state induces via sizeable pd hybridization remarkably strong next-nearest neighbor interactions stabilizing this ordering. The subtle balance of magnetic interactions gives rise to magneto-elastic coupling, explaining pronounced structural anomalies observed at the magnetic ordering transition.

cond-mat.str-el