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Dzyaloshinskii-Moriya interaction (DMI) plays a crucial role to stabilize the exotic topologically stable skyrmion spin-textures in the noncentrosymmetric crystals. The recent discovery of biskyrmions and skyrmions in the globally centrosymmetric crystals has raised debate about the role of the DMI in causing the spin textures, since DMI vanishes in such crystal structures. Theoretical studies, on the other hand, suggest non-vanishing DMI even if there is local inversion symmetry breaking in an otherwise globally centrosymmetric crystal structure. Motivated by such theoretical predictions, we present here the results of a systematic crystal structure study of two skyrmion-hosting Ni2In-type centrosymmetric hexagonal compounds, MnNiGa and MnPtGa, using the atomic pair distribution function (PDF) technique. Our result provides information about structural correlations in the short-range (SR), medium-range (MR) and long-range (LR) regimes simultaneously. The analysis of the experimental PDFs, obtained from high flux, high energy and high-Q synchrotron x-ray powder diffraction patterns, reveal that the local SR structure of both MnNiGa and MnPtGa compounds corresponds to the noncentrosymmetric trigonal space group P3m1, while the structure in the MR+LR regimes remains hexagonal in the centrosymmetric P63/mmc space group. These findings are also supported by theoretical DFT calculations. Our results in conjunction with the previous theoretical predictions, provide a rationale for the genesis of skyrmions in centrosymmetric materials in terms of non-vanishing DMI due to local inversion symmetry breaking. We believe that our findings would encourage a systematic search of skyrmionic textures and other topological phenomena in a vast family of centrosymmetric materials.

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 N\'{e}el 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 $100~\textrm{\r{A}}$, most likely in the form of N\'{e}el-type antiferromagnetic cycloids., Comment: 15 pages, 12 figures

Frustration effects in magnetic systems have traditionally been investigated considering pre-existing site-disorder or lattice geometry of the high-temperature paramagnetic phase. We present here evidence for emergence of geometrical frustration as a function of temperature due to spin canting in the long-range ordered (LRO) ferrimagnetic (FMI) phase of BaFe12O19 (BFO), an M-type hexaferrite of enormous technological applications. Results of neutron scattering and magnetic susceptibility studies on BFO are presented to show for the first time the emergence of highly degenerate kagome spin configuration for the basal plane spin component of BFO with concomitant freezing of transverse and longitudinal components of the spins leading to two spin-glass transitions in coexistence with the LRO FMI phase. Our results mimic the theoretical predictions for concentrated Heisenberg systems even though the source of frustration in BFO is the geometry of the lattice and not site-disorder. We believe that our findings will stimulate theoretical studies to unravel the physics of spin-glass transitions in LRO systems due to emergent geometrical frustration, an aspect that has remained unexplored so far. We also believe that this work will encourage further experimental studies in search of low temperature spin-glass transition(s) in LRO phases of various hexaferrites and even other LRO magnetic compounds with spins arranged on triangular, pyrochlore and spinel lattices without any substitutional disorder.

The availability of large high-quality single crystals is an important prerequisite for many studies in solid-state research. The optical floating-zone technique is an elegant method to grow such crystals, offering potential to prepare samples that may be hardly accessible with other techniques. As elaborated in this report, examples include single crystals with intentional compositional gradients, deliberate off-stoichiometry, or complex metallurgy. For the cubic chiral magnets Mn$_{1-x}$Fe$_{x}$Si and Fe$_{1-x}$Co$_{x}$Si, we prepared single crystals in which the composition was varied during growth from $x = 0 - 0.15$ and from $x = 0.1 - 0.3$, respectively. Such samples allowed us to efficiently study the evolution of the magnetic properties as a function of composition, as demonstrated by means of neutron scattering. For the archetypical chiral magnet MnSi and the itinerant antiferromagnet CrB$_{2}$, we grew single crystals with varying initial manganese (0.99 to 1.04) and boron (1.95 to 2.1) content. Measurements of the low-temperature properties addressed the correlation between magnetic transition temperature and sample quality. Furthermore, we prepared single crystals of the diborides ErB$_{2}$, MnB$_{2}$, and VB$_{2}$. In addition to high vapor pressures, these materials suffer from peritectic formation, potential decomposition, and high melting temperature, respectively., Comment: 16 pages, 13 figures

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.

We have systematically studied the magnetic properties of Cu$_{4-x}$Zn$_x$(OH)$_6$FBr by the neutron diffraction and muon spin rotation and relaxation ($\mu$SR) techniques. Neutron-diffraction measurements suggest that the long-range magnetic order and the orthorhombic nuclear structure in the $x$ = 0 sample can persist up to $x$ = 0.23 and 0.43, respectively. The temperature dependence of the zero-field (ZF) $\mu$SR spectra provide two characteristic temperatures, $T_{A0}$ and $T_{\lambda}$. Comparison between $T_{A0}$ and $T_M$ from previously reported magnetic-susceptibility measurements suggest that the former comes from the short-range interlayer-spin clusters that persist up to $x$ = 0.82. On the other hand, the doping level where $T_{\lambda}$ becomes zero is about 0.66, which is much higher than threshold of the long-range order, i.e., $\sim$ 0.4. Our results suggest that the change in the nuclear structure may alter the spin dynamics of the kagome layers and a gapped quantum-spin-liquid state may exist above $x$ = 0.66 with the perfect kagome planes., Comment: 5 pages, 4 figures

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.

Magnetic frustration in metals is scarce and hard to pinpoint, but exciting due to the possibility of the emergence of fascinating novel phases. The cubic intermetallic compound HoInCu$_4$ with all holmium atoms on an fcc lattice, exhibits partial magnetic frustration, yielding a ground state where half of the Ho moments remain without long-range order, as evidenced by our neutron scattering experiments. The substitution of In with Cd results in HoCdCu$_4$ in a full breakdown of magnetic frustration. Consequently we found a fully ordered magnetic structure in our neutron diffraction experiments. These findings are in agreement with the local energy scales and crystal electric field excitations, which we determined from specific heat and inelastic neutron scattering data. The electronic density of states for the itinerant bands acts as tuning parameter for the ratio between nearest-neighbor and next-nearest-neighbor interactions and thus for magnetic frustration.

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 $\mu$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.

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 $(3.9\pm0.1)~\mu_{\mathrm{B}}/\mathrm{f.u.}$, 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 $\delta \approx 11^{\circ}$, 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., Comment: 14 pages, 15 figures

Barlowite Cu$_4$(OH)$_6$FBr shows three-dimensional (3D) long-range antiferromagnetism, which is fully suppressed in Cu$_3$Zn(OH)$_6$FBr with a kagome quantum spin liquid ground state. Here we report systematic studies on the evolution of magnetism in the Cu$_{4-x}$Zn$_x$(OH)$_{6}$FBr system as a function of $x$ to bridge the two limits of Cu$_4$(OH)$_6$FBr ($x$=0) and Cu$_3$Zn(OH)$_6$FBr ($x$=1). Neutron-diffraction measurements reveal a hexagonal-to-orthorhombic structural change with decreasing temperature in the $x$ = 0 sample. While confirming the 3D antiferromagnetic nature of low-temperature magnetism, the magnetic moments on some Cu$^{2+}$ sites on the kagome planes are found to be vanishingly small, suggesting strong frustration already exists in barlowite. Substitution of interlayer Cu$^{2+}$ with Zn$^{2+}$ with gradually increasing $x$ completely suppresses the bulk magnetic order at around $x$ = 0.4, but leaves a local secondary magnetic order up to $x\sim 0.8$ with a slight decrease in its transition temperature. The high-temperature magnetic susceptibility and specific heat measurements further suggest that the intrinsic magnetic properties of kagome spin liquid planes may already appear from $x>0.3$ samples. Our results reveal that the Cu$_{4-x}$Zn$_x$(OH)$_6$FBr may be the long-thought experimental playground for the systematic investigations of the quantum phase transition from a long-range antiferromagnet to a topologically ordered quantum spin liquid., Comment: 9 pages, 6 figures

We demonstrate that small but finite ferroelectric polarization ($\sim$0.01 $\mu$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., Comment: 12 pages, 8 figures

In this paper, we compare the structural features of Ca modified Ba(Ti, Sn)O3 with that of its Ca-free counterpart to understand why the Ca-modified variant of this lead-free piezoelectric gives a much higher piezoelectric response. We found that in spite of the reduced spontaneous lattice strain, the polarization of the Ca-modified variant is higher. We, therefore, demonstrate that the very large piezoelectric response of (Ba, Ca)(Ti, Sn)O3 is associated with the decoupling of the polarization and lattice strain by Ca-modification., Comment: 26 pages 12 figures

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.

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., Comment: published version + Supplemental material

The existing controversies about the space group symmetries of Pb(ZrxTi1-x)O3 (PZT) above and below antiferrodistortive (AFD) phase transition temperature (TAFD) in the Zr4+- rich (0.620

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.

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., Comment: 12 pages, 6 figures

We have studied the crystal and magnetic structures of Fe-doped hexagonal manganites LuMn1-xFexO3 (x = 0, 0.1, 0.2, and 0.3) by using bulk magnetization and neutron powder diffraction methods. The samples crystalize consistently in a hexagonal structure and maintain the space group P63cm from 2 to 300 K. The N\'eel temperature TN increases continuously with increasing Fe-doping. In contrast to a single {\Gamma}4 representation in LuMnO3, the magnetic ground state of the Fe-doped samples can only be described with a spin configuration described by a mixture of {\Gamma}3 (P63'cm') and {\Gamma}4 (P63'c'm) representations, whose contributions have been quantitatively estimated. The drastic effect of Fe-doping is highlighted by composition-dependent spin reorientations. A phase diagram of the entire composition series is proposed based on the present results and those reported in literature. Our result demonstrates the importance of tailoring compositions in increasing magnetic transition temperatures of multiferroic systems., Comment: 18 pages, 9 figures

A systematic study of the structural, dielectric and piezoelectric behavior of NBT-BT-KNN.

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.

For decades it has been a well-known fact that among the few ferroelectric compounds in the perovskite family namely BaTiO3, KNbO3, PbTiO3 Na1/2Bi1/2TiO3 the dielectric and piezoelectric properties of BaTiO3 is considerably higher than the others in polycrystalline form at room temperature. Further, similar to ferroelectric alloys exhibiting morphotropic phase boundary, single crystals of BaTiO3 exhibits anomalously large piezoelectric response when poled away from the direction of spontaneous polarization at room temperature. These anomalous features in BaTiO3 remained unexplained so far from the structural stand point. In this work we have used high resolution synchrotron X-ray powder diffraction, atomic resolution aberration corrected transmission electron microscopy, in conjunction with a novel powder poling technique, to reveal that (i) the equilibrium state of BaTiO3 is characterized by coexistence of a subtle monoclinic (Mc) phase and tetragonal phase, and (ii) strong electric field induces an orthorhombic phase at 300 K. These results suggest that BaTiO3 at room temperature is within an instability regime, and that this instability is therefore the fundamental factor responsible for the anomalous dielectric and piezoelectric properties of BaTiO3 as compared to the other homologous ferroelectric perovskite compounds. The results demonstrate that pure BaTiO3 at room temperature more akin to lead-based ferroelectric alloys close to the morphotropic phase boundary where polarization rotation and field induced ferroelectric-ferroelectric phase transformations play fundamental role in influencing the piezoelectric behavior., Comment: 24 pages, 9 figures 2 Tables

The coexistence and coupling of magnetic and ferroelectric orderings in single phase multiferroics has evinced enormous scientific interest as it involves breaking of time reversal and space inversion symmetries in the same material. The mutual controllability of the two diverse orderings in multiferroics has potential for developing new generation multifunctional sensor, actuator and data storage devices. We present here evidence for a new exotic facet of multiferroicity, whereby one can raise the strength of antiferromagnetic (AFM) superexchange interaction and hence tune the N\'eel temperature (TN) from ~120K in bulk to ~350K in 18nm size particles by tuning the ferroelectric distortion in the tetragonal phase of multiferroic (1-x)BiFeO3 -xPbTiO3 solid solutions . This observation is unique to multiferroics only as the TN in non-multiferroic AFM oxides decreases with particle size. Our results provide a scientific basis for designing room temperature single phase multiferroics, useful for making multifunctional device operating at room temperature., Comment: 9 pages, 4 figures, 10 pages supplementary information