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Spinon-magnon mixing was recently reported in botallackite Cu$_2$(OH)$_3$Br with a uniaxially compressed triangular lattice of Cu$^{2+}$ quantum spins [Zhang et al., Phys. Rev. Lett. 125, 037204 (2020)]. Its nitrate counterpart rouaite, Cu$_2$(OH)$_3$NO$_3$, has a highly analogous structure and might be expected to exhibit similar physics. To lay a foundation for research on this material, we clarify rouaite's magnetic phase diagram and identify both low-field phases. The low-temperature magnetic state consists of alternating ferro- and antiferromagnetic chains, as in botallackite, but with additional canting, leading to net moments on all chains which rotate from one chain to another to form a 90$^\circ$ cycloidal pattern. The higher-temperature phase is a helical modulation of this order, wherein the spins rotate from one Cu plane to the next. This extends to zero temperature for fields perpendicular to the chains, leading to a set of low-temperature field-induced phase transitions. Rouaite may offer another platform for spinon-magnon mixing, while our results suggest a delicate balance of interactions and high tunability of the magnetism., Comment: 21 pages, 21 figures; CIF files describing the refinements provided as ancillary files

Spontaneous Hall conductivity has recently been reported in the triangular lattice antiferromagnet Co$_{1/3}$TaS$_2$ under a zero magnetic field. This phenomenon originates from the distinctive noncoplanar triple-Q magnetic ground state, possessing uniform real-space Berry curvature characterized by scalar spin chirality. We investigated the physical properties of Co$_{1/3}$TaS$_2$ by judiciously controlling the composition, revealing a drastic change in its bulk properties, even by slight variations in cobalt composition, despite the same crystal structure. For $0.299 < x < 0.325$, Co$_x$TaS$_2$ keeps all the characteristics of the ground state consistent with the previous studies -- two antiferromagnetic phase transitions at $T_{N1}$ and $T_{N2} (< T_{N1})$, a large spontaneous Hall conductivity (${\sigma}_{xy} (H=0)$), and a weak ferromagnetic moment along the c-axis. However, samples with $x > 0.330$ exhibit distinct bulk properties, including the absence of both ${\sigma}_{xy} (H=0)$ and the weak ferromagnetic moment. Our neutron diffraction data reveal that Co$_x$TaS$_2$ with $x > 0.330$ develops coplanar helical magnetic order with $q_{m1} = (1/3, 0, 0)$. This is entirely different from what has been seen in $x < 0.325$, explaining the observed composition dependence., Comment: 15 pages, 4 figures, accepted for publication in Phys. Rev. B

Exploring the uncharacterized magnetic phases of Co$^{2+}$ chain compounds is critical for finding new low-dimensional magnets hosting quantized excitations. We map the unexplored magnetic phases of the Co$^{2+}$ chain compound Li$_2$CoCl$_4$. Magnetometry reveals magnetic ordering below 7 K with a metamagnetic transition near 16.5 kOe and a gradual transition to a field-aligned paramagnetic state above 31 kOe. Curie-Weiss fits to the high temperature susceptibility reveal a high-spin (spin-$\frac{3}{2}$) state for cobalt. Heat capacity data, though, give a magnetic entropy change of 5.46 J/mol, consistent with cobalt effective spin-$\frac{1}{2}$ systems. To characterize the zero-field antiferromagnetic ordering, we separately calculated the energy of proposed magnetic structures with density functional theory and collected 3.5 K neutron diffraction data, finding that Li$_2$CoCl$_4$ has ferromagnetic chains with antiferromagnetic interactions between them. Increasing field rotates these spin chains, producing the antiferromagnetic to intermediate to paramagnetic transition sequence., Comment: 19 pages, 20 figures, 2 tables

We report the successful synthesis of a new 4$d$ based polycrystalline inverse Heusler alloy Fe$_2$RuGe by an arc melting process and have studied in detail its structural, magnetic and transport properties complemented with first principle calculations. X-ray and neutron diffraction, Extended X-ray Absorption Fine Structure and $^{57}$Fe M\"{o}ssbauer spectroscopic studies confirm the single phase nature of the system where the Fe and Ru atoms are randomly distributed in the 4$c$ and 4$d$ Wyckoff positions in a ratio close to 50:50. The formation of the disordered structure is also confirmed by the theoretical energy minimization calculation. Despite the random cross-site disorder of Fe and Ru atoms, magnetic measurements suggest not only a high Curie temperature of $\sim$860\,K, but also a large saturation magnetic moment $\sim$4.9\,$\mu_B$ per formula unit at 5\,K, considerably exceeding the theoretical limit (4\,$\mu_B$ per formula unit) predicted by the Slater-Pauling rule. Only a few Fe-based inverse Heusler alloys are known to exhibit such high Curie temperatures. Neutron diffraction analysis coupled with the isothermal magnetization value indicates that the magnetic moments in Fe$_2$RuGe are associated with Fe-atoms only, which is also confirmed by M\"ossbauer spectrometry. Interestingly, in comparison to the cubic or hexagonal phase of the parent compound, Fe$_3$Ge, the Curie temperature of Fe$_2$RuGe has increased significantly despite the substitution of the nonmagnetic, yet isoelectronic element Ru in this structurally disordered compound. Our theoretical calculation reveals that the large Fe moment ($\sim2.8\mu_B$/Fe) on the 4$b$ site can be attributed to a charge transfer from this Fe site towards its Ru neighbours. Such a substantial increase in magnetic moment due to electron charge transfer has not previously been reported in a Heusler alloy system.

In this work, we report the successful synthesis of a Fe-based novel half-metallic quaternary Heusler alloy FeMnVGa and its structural, magnetic and transport properties probed through different experimental methods and theoretical technique. Density functional theory (DFT) calculations performed on different types of structure reveal that Type-2 ordered structure (space group: F-43m, Ga at 4a, V at 4b, Mn at 4c and Fe at 4d) possess minimum energy among all the ordered variants. Ab-initio simulations in Type 2 ordered structure further reveal that the compound is half-metallic ferromagnet (HMF) having a large spin-polarization (89.9 %). Neutron diffraction reveal that the compound crystalizes in disordered Type-2 structure (space group: Fm-3m) in which Ga occupy at 4a, V at 4b and Fe/Mn occupy 4c/4d sites with 50:50 proportions. The structural disorder is further confirmed by X-ray diffraction (XRD), extended X-ray absorption fine structure (EXAFS),57Fe Mossbauer spectrometry results and DFT calculations. Magnetisation studies suggest that the compound orders ferromagnetically below TC ~ 293 K and the saturation magnetization follows Slater-Pauling rule. Mossbauer spectrometry, along with neutron diffraction suggest that Mn is the major contributor to the total magnetism in the compound consistent with the theoretical calculations. First principle calculations indicate that spin-polarization remain high (81.3 %) even in the presence of such large atomic disorder. The robustness of the HMF property in presence of disorder is a quite unique characteristic over other reported HMF in literature and make this compound quiet promising for spintronics applications.

The triangular lattice antiferromagnet (TLAF) has been the standard paradigm of frustrated magnetism for several decades. The most common magnetic ordering in insulating TLAFs is the 120 structure. However, a new triple-Q chiral ordering can emerge in metallic TLAFs, representing the short wavelength limit of magnetic skyrmion crystals. We report the metallic TLAF Co1/3TaS2 as the first example of tetrahedral triple-Q magnetic ordering with the associated topological Hall effect (non-zero {\sigma}_{xy}(H=0)). We also present a theoretical framework that describes the emergence of this magnetic ground state, which is further supported by the electronic structure measured by angle-resolved photoemission spectroscopy. Additionally, our measurements of the inelastic neutron scattering cross section are consistent with the calculated dynamical structure factor of the tetrahedral triple-Q state., Comment: 23 pages, 4 figures, SI not included. Accepted for publication in Nature Communications

Owing to the geometrical frustration, Mn$_3 $Sn exhibits a 120$^{\circ}$ in-plane triangular antiferromagnetic (AFM) order with a large anomalous Hall effect (AHE). Here, we present a combined theoretical and experimental study to demonstrate that the in-plane AFM structure in Mn$_3 $Sn can be significantly modified to a tunable noncoplanar magnetic state by suitable electron doping. With the help of Density Functional Theory calculations we show that the presence of higher-order exchange interactions in the system leads to the stabilization of the noncoplanar magnetic ground state, which is further established by neutron diffraction study in the Fe-doped Mn$_3 $Sn sample. Interestingly, we find a large scalar spin chirality (SSC) induced topological AHE that can be significantly tuned with the degree of non-coplanarity. We carry out 60~T magnetic and Hall resistivity measurements to demonstrate the contribution of SSC to the observed AHE. We also illustrate a simultaneous manipulation of dual order in the system, where the AHE arising from the in-plane 120$^{\circ}$ triangular AFM order can switch its sign without affecting the AHE generated by the SSC. The present study opens up a new direction to explore novel quantum phenomena associated with the coexistence of multiple orders.

We present studies on crystal structure and ionic diffusion behaviors of superionic Cu$_{2-\delta}$Se ($\delta$=0, 0.04, and 0.2) by utilizing neutron powder diffraction and quasi-elastic neutron scattering. In the superionic phase, the structural model with Cu ions occupying the Wyckoff sites of 8$c$ and 32$f$ provides the best description of the structure. As the content of Cu increasing in Cu$_{2-\delta}$Se, the Cu occupancy increases on the 32$f$ site, but decreases on the 8$c$ site . Fitting to the quasi-elastic neutron scattering spectra reveals two diffusion modes, the localized diffusion between the 8$c$ and 32$f$ sites and the long-range diffusion between the adjacent 8$c$ sites using the 32$f$ site as a bypass, respectively. Between 430 and 650 K, we measured that the compound with more Cu content exhibits a larger long-range diffusion coefficient. Temperature in this range does not affect the long-range diffusion process obviously. Our results suggest the two diffusion modes cooperative and thus provide a microscopic understanding of the ionic diffusion of the Cu ions in superionic Cu$_{2-\delta}$Se., Comment: 6 pages, 3 figures

In frustrated magnetic systems, the competition amongst interactions can introduce extremely high degeneracy and prevent the system from readily selecting a unique ground state. In such cases, the magnetic order is often exquisitely sensitive to the balance among the interactions, allowing tuning among novel magnetically ordered phases. In antlerite, Cu$_3$SO$_4$(OH)$_4$, Cu$^{2+}$ ($S=1/2$) quantum spins populate three-leg zigzag ladders in a highly frustrated quasi-one-dimensional structural motif. We demonstrate that at zero applied field, in addition to its recently reported low-temperature phase of coupled ferromagnetic and antiferromagnetic spin chains, this mineral hosts an incommensurate helical+cycloidal state, an idle-spin state, and a multiple-$q$ phase which is the magnetic analog of misfit crystal structures. The antiferromagnetic order on the central leg is reentrant. The high tunability of the magnetism in antlerite makes it a particularly promising platform for pursuing exotic magnetic order., Comment: 19 pages, 16 Figures, follow-up paper to arXiv:2203.15343. mCIFs describing the magnetic refinements are included as ancillary files

Magnetic properties of the quasicrystal approximant Au$_{65}$Ga$_{21}$Tb$_{14}$ were investigated by the magnetization and the neutron diffraction experiments. The temperature dependences of the magnetic susceptibility and the magnetization curve indicate dominant ferromagnetic interactions, while the whirling antiferromagnetic order was found from the neutron diffraction experiments. In the antiferromagnetic phase, the magnetic moments are aligned almost perpendicular to a pseudo five-fold symmetry axis, which should correspond to the easy-axis direction of a Tb atom. The magnetic properties similar to those of Au$_{72}$Al$_{14}$Tb$_{14}$ in spite of the difference in the electron-per-atom ratio suggest the robustness of the easy-axis anisotropy against the chemical substitution of the nonmagnetic atoms., Comment: 6 pages, 3 figures, 2 tables

Magnetic properties of the pyrovanadate CaCoV$_2$O$_7$ have been studied by means of the bulk magnetization and neutron powder diffraction measurements. Magnetic susceptibility in the paramagnetic phase shows Curie-Weiss behavior with negative Weiss temperature $\Theta \simeq -22.5$ K, indicating dominant antiferromagnetic interactions. At $T_{\rm N} = 3.44$ K, CaCoV$_2$O$_7$ shows antiferromagnetic order, accompanied by a weak net ferromagnetic moment of $\sim 0.05$~$\mu_{\rm B}/{\rm Co}^{2+}$. Neutron powder diffraction confirms the formation of antiferromagnetic order below $T_{\rm N}$. It was further confirmed from the magnetic structure determination that the two Co$^{2+}$ ions in the adjacent edge-sharing octahedra have almost parallel (ferromagnetic) spin arrangement, indicative of a formation of a ferromagnetic spin dimer. The antiferromagnetic order is, in turn, stabilized by sizable inter-dimer antiferromagnetic interactions.

Dimensionality is a critical factor in determining the properties of solids and is an apparent built-in character of the crystal structure. However, it can be an emergent and tunable property in geometrically frustrated spin systems. Here, we study the spin dynamics of the tetrahedral cluster antiferromagnet, pharmacosiderite, via muon spin resonance and neutron scattering. We find that the spin correlation exhibits a two-dimensional characteristic despite the isotropic connectivity of tetrahedral clusters made of spin 5/2 Fe3+ ions in the three-dimensional cubic crystal, which we ascribe to two-dimensionalisation by geometrical frustration based on spin wave calculations. Moreover, we suggest that even one-dimensionalisation occurs in the decoupled layers, generating low-energy and one-dimensional excitation modes, causing large spin fluctuation in the classical spin system. Pharmacosiderite facilitates studying the emergence of low-dimensionality and manipulating anisotropic responses arising from the dimensionality using an external magnetic field., Comment: 22 pages, 22 figures

Two-dimensional (2D) layered magnetic materials are generating a great amount of interest for the next generation of electronic devices thanks to their remarkable properties associated to spin dynamics. The recently discovered layered VI$_3$ ferromagnetic phase belongs to this family, although a full understanding of its properties is limited by an ill-defined crystallographic structure. This is not any longer true. Here, we investigate the VI$_3$ crystal structure upon cooling using both synchrotron X-ray and neutron powder diffraction and provide structural models for the two structural transitions occurring at 76 K and 32 K. Moreover, we confirm by magnetic measurements that VI$_3$ becomes ferromagnetic at 50 K and discuss the difficulty of solving its full magnetic structure by neutrons. We equally determined the magnetic properties of our recently reported LiVI$_3$ phase, which is alike the well-known CrI$_3$ ferromagnetic phase in terms of electronic and crystallographic structures and found to our surprise an antiferromagnetic behavior with a N\'eel temperature of 12 K. Such a finding provides extra clues for a better understanding of magnetism in these low dimension compounds. Finally, the easiness of preparing novel Li-based 2D magnetic materials by chemical/electrochemical means opens wide the opportunity to design materials with exotic properties.

The effect of chemical substitution on the ground state of the geometrically frustrated antiferromagnet CsCrF$_4$ has been investigated through a neutron powder diffraction experiment. Magnetic Fe-substituted CsCr$_{0.94}$Fe$_{0.06}$F$_{4}$ and nonmagnetic Al-substituted CsCr$_{0.98}$Al$_{0.02}$F$_{4}$ samples are measured, and magnetic Bragg peaks are clearly observed in both samples. Magnetic structure analysis revealed a 120$^{\circ}$ structure having a magnetic propagation vector $\mathbf{k}_{\rm mag}=(0,0,1/2)$ in CsCr$_{0.94}$Fe$_{0.06}$F$_{4}$. For CsCr$_{0.98}$Al$_{0.02}$F$_{4}$, a quasi-120$^{\circ}$ structure having $\mathbf{k}_{\rm mag}=(1/2,0,1/2)$ is formed. It is notable that the identified magnetic structure in CsCr$_{0.94}$Fe$_{0.06}$F$_{4}$ belongs to a different phase of ground states from those in CsCr$_{0.98}$Al$_{0.02}$F$_{4}$ and the parent CsCrF$_{4}$. These results suggest that the Fe-substitution strongly influences the ground state of CsCrF$_{4}$.

We report the magnetic structure of room-temperature-stable, monoclinic Mn$_3$As$_2$ at 3 K and 250 K using neutron powder diffraction measurements. From magnetometry data, the Curie temperature of Mn$_3$As$_2$ was confirmed to be around 270 K. Calorimetry analysis showed the presence of another transition at 225 K. At 270 K, Mn$_3$As$_2$ undergoes a $k = 0$ ferrimagnetic ordering in the magnetic space group $C2/m$ (#12.58) with Mn moments pointing along $b$. Below 225 K, there is a canting of Mn moments in the $ac$ plane which produces a multi-$k$ non-collinear magnetic structure in space group $C2/c$ (#15.85). The components of Mn moments along $b$ follow $k=0$ ordering and the components along $a$ and $c$ have $k = [0 0 \frac{1}{2}]$ propagation vector. The change in the magnetic ground state with temperature provides a deeper insight into the factors that govern magnetic ordering in Mn-As compounds., Comment: 6 pages, 6 figures, 1 table

Low thermal conductivity is favorable for preserving the temperature gradient between the two ends of a thermoelectric material in order to ensure continuous electron current generation. In high-performance thermoelectric materials, there are two main low thermal conductivity mechanisms: the phonon anharmonic in PbTe and SnSe and phonon scattering resulting from the dynamic disorder in AgCrSe2 and CuCrSe2, which have been successfully revealed by inelastic neutron scattering. Using neutron scattering and ab initio calculations, we report here a mechanism of static local structure distortion combined with phonon-anharmonic-induced ultralow lattice thermal conductivity in {\alpha}-MgAgSb. Since the transverse acoustic phonons are almost fully scattered by the compound's intrinsic distorted rocksalt sublattice, the heat is mainly transported by the longitudinal acoustic phonons. The ultralow thermal conductivity in {\alpha}-MgAgSb is attributed to its atomic dynamics being altered by the structure distortion, which presents a possible microscopic route to enhance the performance of similar thermoelectric materials., Comment: 43 pages, 5 figures

We investigate the nonequilibrium pair density wave order parameter in a simple microscopic model with the ground state $d-$ wave spatially uniform superconductivity. After pushing the system out of equilibrium by a short-time induced order parameter, the system can exhibit robust free nondecaying oscillations of nonuniform superconducting order. In the weak nonequilibrium regime, the frequency of these oscillations is about $2\Delta/\hbar$ and the amplitude can be explained qualitatively by features of equilibrium free energy. In case when the system was taken far from equilibrium, it transits to a non-linear regime where even metastable coexistence of $d-$ wave superconducting and pair density wave gaps are possible.

Doped BaCoSO was recently predicted to be a high-temperature superconductor in a new class based on Co and Ni. Using a Co-S self flux method, we synthesized single crystals of the antiferromagnetic insulator BaCoSO. Our magnetic and specific heat measurements and neutron diffraction provide details of its magnetic anisotropy and order. Its band gap was determined to be about 1.3 eV by our measurements of its photoemission spectrum and infrared optical conductivity. Our results can pave the way to exploring the predicted superconductivity in this Co-based material., Comment: 6 pages, 6 figures and Supplemental Material

Neutron powder diffraction experiment has been performed on the quasicrystal approximant Au$_{72}$Al$_{14}$Tb$_{14}$, a body-center-cubic crystal of icosahedral spin clusters. The long-range antiferromagnetic order was confirmed at the transition temperature $T_{\rm N} = 10.4$ K. The magnetic structure consists of noncoplanar whirling spins on the icosahedral clusters, arranging antiferroic-manner. A simple icosahedral spin-cluster model with uniaxial anisotropy accounts well the whirling spin order as well as the in-field metamagnetic transition, indicating that the icosahedral symmetry is essential., Comment: 6 pages, 4 figures

The crystal structure and magnetic properties of the spin-1 triangular-lattice antiferromagnet Ba$_2$La$_2$NiTe$_2$O$_{12}$ are reported. Its crystal structure is trigonal $R\bar{3}$, which is the same as that of Ba$_2$La$_2$NiW$_2$O$_{12}$ [Y. Doi et al., J. Phys.: Condens. Matter 29, 365802 (2017)]. However, the exchange interaction $J/k_{\mathrm{B}}\simeq19$ K is much greater than that observed in the tungsten system. At zero magnetic field, Ba$_2$La$_2$NiTe$_2$O$_{12}$ undergoes successive magnetic phase transitions at $T_{\mathrm{N}1}=9.8$ K and $T_{\mathrm{N}2}=8.9$ K. The ground state is accompanied by a weak ferromagnetic moment. These results indicate that the ground-state spin structure is a triangular structure in a plane perpendicular to the triangular lattice owing to the small easy-axis-type anisotropy. The magnetization curve exhibits the one-third plateau characteristic of a two-dimensional triangular-lattice Heisenberg-like antiferromagnet. Exchange constants are also evaluated using density functional theory (DFT). The DFT results demonstrate the large difference in the exchange constants between tellurium and tungsten systems and the good two-dimensionality of the tellurium system., Comment: 12 pages, 15 figures, 4 tables

In an ideal classical pyrochlore antiferromagnet without perturbations, an infinite degeneracy at a ground state leads to absence of a magnetic order and spin-glass transition. Here we present Na$_3$Mn(CO$_3$)$_2$Cl as a new candidate compound where classical spins are coupled antiferromagnetically on the pyrochlore lattice, and report its structural and magnetic properties.The temperature dependences of the magnetic susceptibility and heat capacity, and the magnetization curve are consistent with those of an $S$ = 5/2 pyrochlore lattice antiferromagnet with nearest-neighbor interactions of 2 K. Neither an apparent signature of a spin-glass transition nor a magnetic order is detected in magnetization and heat capacity measurements, or powder neutron diffraction experiments. On the other hand, an antiferromagnetic short-range order from the nearest neighbors is evidenced by the $Q$-dependence of the diffuse scattering which develops around 0.85 \AA$^{-1}$. A high degeneracy near the ground state in Na$_3$Mn(CO$_3$)$_2$Cl is supported by the magnetic entropy estimated as almost 4 J K$^{-2}$ mol$^{-1}$ at 0.5 K., Comment: 9 pages, 7 figures, accepted to PRB