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We present a comprehensive study of the structural, magnetic, and thermodynamic properties, as well as the adiabatic demagnetization refrigeration (ADR) performance of NaGdP$_2$O$_7$. Although NaGdP$_2$O$_7$ exhibits antiferromagnetic ordering at a N\'eel temperature of $T_{\rm N} = 570$ mK in zero field, ADR experiments achieved a minimum temperature of 220 mK starting from $T = 2$ K under an applied magnetic field of $\mu_0H = 5$ T. The warm-up time back to $T = 2$ K exceeds 60 hours, which is roughly 50 times longer than that of its Yb-based analogue, underscoring the potential of NaGdP$_2$O$_7$ as an efficient precooling stage in double-stage ADR systems. We show that NaGdP$_2$O$_7$ can be seen as a network of ferromagnetic spin chains with antiferromagnetic interchain couplings and also investigate the influence of antiferromagnetic ordering on the magnetic entropy. We find that the temperature dependence of the entropy plays a more dominant role than its magnetic field dependence in the magnetically ordered state., Comment: 10 pages, 6 figures

We use magnetization measurements under pressure along with \textit{ab initio} and cluster many-body calculations to investigate magnetism of the Kitaev candidate Li$_2$RhO$_3$. Hydrostatic compression to 4.2~GPa leads to a decrease in the magnitude of the ferromagnetic Kitaev coupling $K$ and the corresponding increase in the off-diagonal anisotropy $\Gamma$, whereas the experimental Curie-Weiss temperature changes from negative to positive with the slope of +40~K/GPa. On the other hand, spin freezing persists up to at least 3.25~GPa with the almost constant freezing temperature of $5.5-6.0$~K that does not follow the large changes in the exchange couplings and indicates the likely extrinsic origin of spin freezing. Magnetic frustration in Li$_2$RhO$_3$ is mainly related to the interplay between ferromagnetic $K$ and antiferromagnetic $\Gamma$, along with the weakness of the third-neighbor coupling $J_3$ that would otherwise stabilize zigzag order. The small $J_3\simeq 0.1$\,meV distinguishes Li$_2$RhO$_3$ from other Kitaev candidates., Comment: Main text: 8 pages, 6 figures. Supplemental material: 3 pages, 2 figures

Presence of magnetism in potentially altermagnetic RuO$_2$ has been a subject of intense debate. Using broadband infrared spectroscopy combined with density-functional band-structure calculations, we show that optical conductivity of RuO$_2$, the bulk probe of its electronic structure, is well described by the nonmagnetic model of this material. The sharp Pauli edge demonstrates the presence of a Dirac nodal line lying 45 meV below the Fermi level. Good match between the experimental and ab initio plasma frequencies underpins weakness of electronic correlations. The intraband part of the optical conductivity indicates Fermi-liquid behavior with two distinct scattering rates below 150 K. Fermi-liquid theory also accounts for the temperature-dependent magnetic susceptibility of RuO$_2$ and allows a consistent description of this material as paramagnetic metal., Comment: Main text + Supplementary

Trillium lattices formed by corner-shared triangular units are the platform for magnetic frustration in three dimensions. Herein, we report structural and magnetic properties of the Cr-based double trillium lattice material KBaCr$_2$(PO$_4$)$_3$ studied by x-ray diffraction, magnetization, heat capacity, thermal conductivity, and $^{31}$P nuclear magnetic resonance (NMR) measurements complemented by density-functional band-structure calculations. Heat capacity and $^{31}$P NMR measurements reveal the magnetic transition at $T_{\rm N1} \simeq 13.5$ K in zero field followed by another transition at $T_{\rm N2} \simeq 7$ K in weak applied fields. The NMR sublattice magnetization confirms that the transition at $T_{\rm N1}$ is 3D in nature. The $^{31}$P spin-lattice relaxation rate in the ordered state follows the $T^3$ behavior indicative of the two-magnon Raman process. The spin lattice of KBaCr$_2$(PO$_4$)$_3$ comprises two crystallographically nonequivalent ferromagnetic sublattices that are coupled antiferromagnetically, thus eliminating frustration in this trillium network., Comment: 12 pages, 13 figures

A detailed study of the structural and magnetic properties of the spin-$3/2$ hyperkagome lattice compound Li$_2$MgMn$_3$O$_8$ is reported. This material shows ferromagnetic response below $T_{\rm C} \simeq 20.6$ K, the temperature almost three times lower than the Curie-Weiss temperature $\theta_{\rm CW} \simeq 56.6$ K. Density-functional band-structure calculations suggest that this reduction in $T_{\rm C}$ may be caused by long-range antiferromagnetic couplings that frustrate nearest-neighbor ferromagnetic couplings on the hyperkagome lattice. Large magnetocaloric effect is observed around the $T_{\rm C}$ with a maximum value of isothermal entropy change $\Delta S_{\rm m}\simeq 20$ J/kg-K and a maximum relative cooling power of $RCP\simeq 840$ J/kg for the 7 T magnetic field change. Critical analysis of the magnetization data and scaling analysis of the magnetocaloric effect suggest the 3D Heisenberg/XY universality class of the transition. The DC and AC magnetization measurements further reveal glassy nature of the ferromagnetic transition. A detailed study of the non-equilibrium dynamics via magnetic relaxation and memory effect measurements demonstrates that the system evolves through a large number of intermediate metastable states and manifests significant memory effect in the cluster-glass state., Comment: 17 pages, 14 figures

We report temperature-dependent reflectivity spectra of the layered van der Waals magnet CrSBr in the far-infrared region. Polarization-dependent measurements resolve the vibrational modes along the E$\|a$- and $b$-axes and reveal the clear structural anisotropy. While the $a$-axis phonons notably harden on cooling, the $b$-axis phonon frequencies are almost temperature-independent. A phonon splitting due to the antiferromagnetic phase transition is observed for the 180~cm$^{-1}$ $a$-axis vibrational mode, accompanied by a phonon softening below $T_N$. Furthermore, an additional mode with strong magnetic characteristics at $\sim$360~cm$^{-1}$ is identified and attributed to the magnon excitation of CrSBr., Comment: 6 pages, 3 figures

Magnetic materials are composed of the simple building blocks of magnetic moments on a crystal lattice that interact via magnetic exchange. Yet from this simplicity emerges a remarkable diversity of magnetic states. Some reveal the deep quantum mechanical origins of magnetism, for example, quantum spin liquid (QSL) states in which magnetic moments remain disordered at low temperatures despite being strongly correlated through quantum entanglement. A promising theoretical model of a QSL is the Kitaev model, composed of unusual bond-dependent exchange interactions, but experimentally, this model is challenging to realise. Here we show that the material requirements for the Kitaev QSL survive an extended pseudo-edge-sharing superexchange pathway of Ru3+ octahedra within the honeycomb layers of the inorganic framework solid, RuP3SiO11. We confirm the requisite jeff = 1/2 state of Ru3+ in RuP3SiO11 and resolve the hierarchy of exchange interactions that provide experimental access to an unexplored region of the Kitaev model., Comment: 28 Pages, 5 figures, 1 table

Pressure evolution of the crystal structure and magnetism of the honeycomb $\alpha$-RuBr$_3$ is studied using high-pressure x-ray diffraction, magnetometry, and density-functional band-structure calculations. Hydrostatic compression transforms antiferromagnetic $\alpha$-RuBr$_3$ ($R\bar 3$) into paramagnetic $\alpha'$-RuBr$_3$ ($P\bar 1$) where short Ru-Ru bonds cause magnetism collapse above 1.3 GPa at 0 K and 2.5 GPa at 295 K. Below this critical pressure, the N\'eel temperature of $\alpha$-RuBr$_3$ increases with the slope of 1.8 K/GPa. Pressure tunes $\alpha$-RuBr$_3$ away from the Kitaev limit, whereas increased third-neighbor in-plane coupling and interlayer coupling lead to a further stabilization of the collinear zigzag state. Both $\alpha$- and $\alpha'$-RuBr$_3$ are metastable at ambient pressure, but their transformation into the thermodynamically stable $\beta$-polymorph is kinetically hindered at room temperature., Comment: 8 pages + Supplemental Material: published version

We use magnetometry, calorimetry, and high-resolution capacitive dilatometry, as well as single-crystal neutron diffraction to explore temperature-field phase diagram of the anisotropic honeycomb magnet BaCo$_2$(AsO$_4)_2$. Our data reveal four distinct ordered states observed for in-plane magnetic fields. Of particular interest is the narrow region between 0.51 and 0.55 T that separates the up-up-down order from the fully polarized state and coincides with the field range where signatures of the spin-liquid behavior have been reported. We show that magnetic Bragg peaks persist in this intermediate phase, thus ruling out its spin-liquid nature. However, the simultaneous nonmonotonic evolution of nuclear Bragg peaks suggests the involvement of the lattice, witnessed also in other regions of the phase diagram where large changes in the sample length are observed upon entering the magnetically ordered states. Our data highlight the importance of lattice effects in BaCo$_2$(AsO$_4)_2$.

A detailed study of the magnetic and magnetocaloric properties of a garnet compound Mn$_{3}$Cr$_{2}$Ge$_{3}$O$_{12}$ is carried out using x-ray diffraction, magnetization, heat capacity, and neutron diffraction measurements as well as \textit{ab initio} band-structure calculations. This compound manifests two successive magnetic transitions at $T_{\rm N1} \simeq 4.5$ K and $T_{\rm N2} \simeq 2.7$ K. Neutron powder diffraction experiments reveal that these two transitions correspond to the collinear and non-collinear antiferromagnetic ordering of the nonfrustrated Cr$^{3+}$ and frustrated Mn$^{2+}$ sublattices, respectively. The interactions within each of the Cr and Mn sublattices are antiferromagnetic, while the inter-sublattice interactions are ferromagnetic. The $H-T$ phase diagram is quite complex and displays multiple phases under magnetic field, which can be attributed to the frustrated nature of the spin lattice. Mn$_{3}$Cr$_{2}$Ge$_{3}$O$_{12}$ shows a large magnetocaloric effect with a maximum value of isothermal entropy change $\Delta S_{\rm m} \simeq -23$ J/kg-K and adiabatic temperature change $\Delta T_{\rm ad} \simeq 9$ K for a field change of 7 T. Further, a large value of the relative cooling power ($RCP \simeq 360$ J/kg) demonstrates the promise of using this compound in magnetic refrigeration., Comment: Phys. Rev. B (Accepted) 12 pages, 10 figures, 54 references

The properties of kagome metals are governed by the interdependence of band topology and electronic correlations resulting in remarkably rich phase diagrams. Here, we study the temperature evolution of the bulk electronic structure of the antiferromagnetic kagome metal FeGe using infrared spectroscopy. We uncover drastic changes in the low-energy interband absorption at the 100 K structural phase transition that has been linked to a charge-density-wave (CDW) instability. We explain this effect by the minuscule Fe displacement in the kagome plane, which results in parallel bands in the vicinity of the Fermi level. In contrast to conventional CDW materials, however, the spectral weight shifts to low energies, ruling out the opening of a CDW gap in FeGe.

We probe the magnetic field-induced Tomonaga-Luttinger liquid (TLL) state in the bond-alternating spin-$1/2$ antiferromagnetic (AFM) chain compound NaVOPO$_4$ using thermodynamic as well as local $\mu$SR and $^{31}$P NMR probes down to milli-K temperatures in magnetic fields up to 14~T. The $\mu$SR and NMR relaxation rates in the gapless TLL regime decay slowly following characteristic power-law behaviour, enabling us to directly determine the interaction parameter $K$ as a function of the magnetic field. These estimates are cross-checked using magnetization and specific heat data. The field-dependent $K$ lies in the range of $0.4 < K < 1$ and indicates repulsive nature of interactions between the spinless fermions, in line with the theoretical predictions. This renders NaVOPO$_4$ the first experimental realization of TLL with repulsive fermionic interactions in hitherto studied $S=1/2$ bond-alternating AFM-AFM chain compounds., Comment: 7 pages, 2 figures, 47 references

Incommensurate magnetic order in the spin-3/2 antiferromagnet Na$_3$RuO$_4$ is uncovered by neutron diffraction combined with ab initio calculations. The crystal structure of Na$_3$RuO$_4$ contains two triangular motifs on different length scales. The magnetic Ru$^{5+}$ ions form a lozenge (diamond) configuration, with tetramers composed of two isosceles triangles. These tetramers are further arranged in layers, such that an effective triangular lattice is formed. The tetramers are nearly antiferromagnetic but frustration between them leads to an incommensurately modulated magnetic structure described by the propagation vector $\vec{k}=(0.242(1), 0, 0.313(1))$. We show that the long-range Ru-O-O-Ru couplings between the tetramers play a major role in Na$_3$RuO$_4$ and suggest an effective description in terms of the spatially anisotropic triangular lattice if the tetramers are treated as single sites., Comment: 8 pages, 8 figures; published version

We present a theoretical study of dolerophanite Cu$_2$OSO$_4$, a layered kagome-like spin-$\frac{1}{2}$ magnetic insulator that can be described either as a system of chains coupled through dimers or as a kagome lattice where every third spin is replaced by a ferromagnetic spin dimer. Building on insights from ab initio calculations, classical numerical minimizations, and semiclassical expansions, we arrive at a minimal microscopic description that accounts for the experimental data reported so far, including the nature of the magnetic order, the reported spin length, and the observed anisotropy. The latter arises by a peculiar competition between the antisymmetric (Dzyaloshinskii-Moriya) and the symmetric part of the exchange anisotropy, which gives rise to a two-step re-orientation process involving two successive continuous phase transitions. Our work uncovers mechanisms stabilizing canted ferrimagnetic order in kagome systems, and highlights strong magnetic anisotropy in the presence if dissimilar magnetic orbitals on crystallographically nonequivalent Cu sites. We also show how these anisotropy terms affect the spin-wave spectrum and how they can be tracked experimentally., Comment: 20 pages, 7 figures

Temperature- and fluence-dependent carrier dynamics of the magnetic Kagome metal Fe$_3$Sn$_2$ were studied using the ultrafast optical pump-probe technique. Two carrier relaxation processes ($\tau_1$ and $\tau_2$) and a laser induced coherent optical phonon were observed. By using the two-temperature model for metals, we ascribe the shorter relaxation $\tau_1$ (~1 ps) to hot electrons transferring their energy to the crystal lattice via electron-phonon scattering. $\tau_2$ (~25 ps), on the other hand, cannot be explained as a conventional process and is attributed to the unconventional (localized) carriers in the material. The observed coherent oscillation is assigned to be a totally symmetric A$_{1g}$ optical phonon dominated by Sn displacements out of the Kagome planes, and possesses a prominently large amplitude, on the order of 10$^{-3}$, comparable to the maximum of the reflectivity change ($\Delta$R/R). This amplitude is equivalent to charge-density-wave (CDW) systems, although no signs of such an instability were hitherto reported in Fe$_3$Sn$_2$. Our results set an unexpected connection between Fe$_3$Sn$_2$ and kagome metals with CDW instabilities, and suggest a unique interplay between phonon and electron dynamics in this compound., Comment: 12 pages, 14 figures

We delineate quantum magnetism in the strongly spin-orbit coupled, distorted honeycomb-lattice antiferromagnet BiYbGeO$_{5}$. Our magnetization and heat capacity measurements reveal that its low-temperature behavior is well described by an effective $J_{\rm eff}=1/2$ Kramers doublet of Yb$^{3+}$. The ground state is nonmagnetic with a tiny spin gap. Temperature-dependent magnetic susceptibility, magnetization isotherm, and heat capacity could be modeled well assuming isolated spin dimers with anisotropic exchange interactions $J_{\rm Z} \simeq 2.6$~K and $J_{\rm XY} \simeq 1.3$~K. Heat capacity measurements backed by muon spin relaxation suggest the absence of magnetic long-range order down to at least 80\,mK both in zero field and in applied fields. This sets BiYbGeO$_5$ apart from Yb$_2$Si$_2$O$_7$ with its unusual regime of magnon Bose-Einstein condensation and suggests negligible interdimer couplings, despite only a weak structural deformation of the honeycomb lattice., Comment: 6 pages, 5 figures

Single-crystal growth, magnetic properties, and magnetocaloric effect of the $S = 3/2$ kagome ferromagnet Li$_9$Cr$_3$(P$_2$O$_7$)$_3$(PO$_4$)$_2$ (trigonal, space group: $P\bar{3}c1$) are reported. Magnetization data suggest dominant ferromagnetic intra-plane coupling with a weak anisotropy and the onset of ferromagnetic ordering at $T_{\rm C} \simeq 2.6$ K. Microscopic analysis reveals a very small ratio of interlayer to intralayer ferromagnetic couplings ($J_{\perp}/J \simeq 0.02$). Electron spin resonance data suggest the presence of short-range correlations above $T_{\rm C}$ and confirms quasi-two-dimensional character of the spin system. A large magnetocaloric effect characterized by isothermal entropy change of $-\Delta S_{\rm m}\simeq 31$ J kg$^{-1}$ K$^{-1}$ and adiabatic temperature change of $-\Delta T_{\rm ad}\simeq 9$ K upon a field sweep of 7 T is observed around $T_{\rm C}$. This leads to a large relative cooling power of $RCP \simeq 284$ J kg$^{-1}$. The large magnetocaloric effect, together with negligible hysteresis render Li$_9$Cr$_3$(P$_2$O$_7$)$_3$(PO$_4$)$_2$ a promising material for magnetic refrigeration at low temperatures. The magnetocrystalline anisotropy constant $K \simeq -7.42 \times 10^4$ erg cm$^{-3}$ implies that the compound is an easy-plane type ferromagnet with the hard axis normal to the $ab$-plane, consistent with the magnetization data., Comment: 13 pages, 14 figures

The coexistence of the charge-density wave (CDW) and superconducting phases and their tunability under external pressure remains one of the key points in understanding the electronic structure of $A$V$_3$Sb$_5$ ($A$ = K, Rb, Cs) kagome metals. Here, we employ synchrotron-based infrared spectroscopy assisted by density-functional calculations to study the pressure evolution of the electronic structure at room temperature up to 17 GPa experimentally. The optical spectrum of CsV$_3$Sb$_5$ is characterized by the presence of localized carriers seen as a broad peak at finite frequencies in addition to the conventional metallic Drude response. The pressure dependence of this low-energy peak reflects the re-entrant behavior of superconductivity and may be interpreted in terms of electron-phonon coupling, varying with the growth and shrinkage of the Fermi surface. Moreover, drastic modifications in the low-energy interband absorptions are observed upon the suppression of CDW. These changes are related to the upward shift of the Sb2 $p_x+p_y$ band that eliminates part of the Fermi surface around the $M$-point, whereas band saddle points do not move significantly. These observations shed new light on the mixed electronic and lattice origin of the CDW in CsV$_3$Sb$_5$.

We report crystal structure and magnetic behavior of the triangular antiferromagnet KYbO$_2$, the A-site substituted version of the quantum spin liquid candidate NaYbO$_2$. The replacement of Na by K introduces an anisotropic tensile strain with 1.6% in-plane and 12.1% out-of-plane lattice expansion. Compared to NaYbO$_2$, both Curie-Weiss temperature and saturation field are reduced by about 20% as the result of the increased Yb--O--Yb angles, whereas the $g$-tensor of Yb$^{3+}$ becomes isotropic with $g=3.08(3)$. Field-dependent magnetization shows the plateau at 1/2 of the saturated value and suggests the formation of the up-up-up-down field-induced order in the triangular AYbO$_2$ oxides (A = alkali metal), in contrast to the isostructural selenides that exhibit the 1/3 plateau and the up-up-down field-induced order.

We present a temperature-dependent infrared spectroscopy study on the layered topological semimetal Nb$_3$SiTe$_6$ combined with density-functional theory (DFT) calculations of the electronic band structure and optical conductivity. Our results reveal an anisotropic behavior of the in-plane ($ac$-plane) optical conductivity, with three pronounced excitations located at around 0.15, 0.28, and 0.41~eV for the polarization of the incident radiation along the $c$ axis. These excitations are well reproduced in the theoretical spectra. Based on the \textit{ab initio} results, the excitations around 0.15 eV and 0.28 eV are interpreted as fingerprints of van Hove singularities in the electronic band structure and compared to the findings for other topological semimetals., Comment: 9 pages, 7 figures, accepted for publication in Phys. Rev. B

Crystal structure, thermodynamic properties, and adiabatic demagnetization refrigeration (ADR) effect in the spin-7/2 triangular antiferromagnet KBaGd(BO3)2 are reported. With the average nearest-neighbor exchange coupling of 44 mK, this compound shows magnetic order below $T_N = 263$\,mK in zero field. The ADR tests reach the temperature of $T_{min} = 122$ mK, more than twice lower than $T_N$, along with the entropy storage capacity of 192 mJK$^{-1}$cm$^{-3}$ and the hold time of more than 8 hours in the PPMS setup, both significantly improved compared to the spin-1/2 Yb$^{3+}$ analog. We argue that KBaGd(BO3)2 shows a balanced interplay of exchange and dipolar couplings that together with structural randomness and geometrical frustration shift $T_{min}$ to well below the ordering temperature $T_N$, therefore facilitating the cooling., Comment: 8 pages, 6 figures, minor changes to the previous version, accepted for publication in Phys. Rev. B

The 1111 compounds with an alternating sequence of fluorite and antifluorite layers serve as structural hosts for the vast family of Fe-based superconductors. Here, we use neutron powder diffraction and density-functional-theory (DFT) band-structure calculations to study magnetic order of Eu2+ in the [EuF]+ fluorite layers depending on the nature of the [TAs]- antifluorite layer that can be non-magnetic semiconducting (T = Zn), magnetic semiconducting (T = Mn), or magnetic metallic (T = Fe). Antiferromagnetic transitions at TN ~ 2.4 - 3 K due to an ordering of the Eu2+ magnetic moments were confirmed in all three EuTAsF compounds. Whereas in EuTAsF (T = Zn and Mn), the commensurate k1 = (1/2 1/2 0) stripe order pattern with magnetic moments within the ab-plane is observed, the order in EuFeAsF is incommensurate with k = (0 0.961(1) 1/2) and represents a cycloid of Eu2+ magnetic moments confined within the bc-plane. Additionally, the Mn2+ sublattice in EuMnAsF features a robust G-type antiferromagnetic order that persists at least up to room temperature, with magnetic moments along the c-direction. Although DFT calculations suggest stripe antiferromagnetic order in the Fe-sublattice of EuFeAsF as the ground state, neutron diffraction reveals no evidence of long-range magnetic order associated with Fe. We show that the frustrating interplane interaction J3 between the adjacent [EuF]+ layers is comparable with in-plane J1-J2 interactions already in the case of semiconducting fluorite layers [TAs]- (T = Zn and Mn) and becomes dominant in the case of the metallic [FeAs]- ones. The latter, along with a slight orthorhombic distortion, is proposed to be the origin of the incommensurate magnetic structure observed in EuFeAsF.

Deep neural networks (DNNs) are often used for text classification tasks as they usually achieve high levels of accuracy. However, DNNs can be computationally intensive with billions of parameters and large amounts of labeled data, which can make them expensive to use, to optimize and to transfer to out-of-distribution (OOD) cases in practice. In this paper, we propose a non-parametric alternative to DNNs that's easy, light-weight and universal in text classification: a combination of a simple compressor like gzip with a $k$-nearest-neighbor classifier. Without any training, pre-training or fine-tuning, our method achieves results that are competitive with non-pretrained deep learning methods on six in-distributed datasets. It even outperforms BERT on all five OOD datasets, including four low-resource languages. Our method also performs particularly well in few-shot settings where labeled data are too scarce for DNNs to achieve a satisfying accuracy.

We have synthesized single-crystal samples of $\beta$-VOSO$_4$ and fully characterized their magnetic properties. Our magnetic susceptibility, high field magnetization and powder inelastic neutron scattering results are in excellent agreement with theoretical expressions for a one-dimensional spin-1/2 Heisenberg chain with an exchange parameter of $3.83(2)$ meV. Ab initio calculations identify the superexchange pathway, revealing that the spin-chain does not run along the expected crystallographic chain $a$ direction but instead between V$^{4+}$O$_{6}$ octahedra that are linked via SO$_{4}$ tetrahedra along the $b$ axis. We do not detect any phase transition to a long-range magnetic order within our experimental conditions, indicating $\beta$-VOSO$_4$ is very close to an ideal one-dimensional magnetic system.

Kagome metals possess peculiar optical spectra consisting of contributions from free charge carriers in a Drude-type response, localized carriers seen as a strongly temperature-dependent localization peak, and, in some cases, phonons displaying strong anomalies. The rare-earth kagome metal series, $R$Mn$_6$Sn$_6$, provides a marvelous playground to study the electronic properties of kagome metals in the presence of variable magnetic order. Here, we report temperature-dependent reflectivity studies on two members of the $R$Mn$_6$Sn$_6$ family, GdMn$_6$Sn$_6$ (in-plane ferrimagnet) and TbMn$_6$Sn$_6$ (out-of-plane ferrimagnet), in a broad energy range (50 - 18000 cm$^{-1}$, equivalent to 6.2 meV - 2.23 eV) down to 10 K. At high temperatures, a phonon mode at approximately 160 cm$^{-1}$ is observed, which becomes screened out in TbMn$_6$Sn$_6$ below $\sim$ 150 K as the localization peak linearly passes through the mode. In GdMn$_6$Sn$_6$, the disappearance of the phonon is accompanied by the onset of saturation of the peak position, suggesting an unusual interplay between the two features., Comment: 7 pages, 3 figures

The mixed-valent iridate Ba3InIr2O9 has been discussed as a promising candidate for quantum spin-liquid behavior. The compound exhibits Ir$^{4.5+}$ ions in face-sharing IrO6 octahedra forming Ir2O9 dimers with three t2g holes per dimer. Our results establish Ba3InIr2O9 as a cluster Mott insulator. Strong intra-dimer hopping delocalizes the three t2g holes in quasi-molecular dimer states while inter-dimer charge fluctuations are suppressed by Coulomb repulsion. The magnetism of Ba3InIr2O9 emerges from spin-orbit entangled quasi-molecular moments with yet unexplored interactions, opening up a new route to unconventional magnetic properties of 5d compounds. Using single-crystal x-ray diffraction we find the monoclinic space group C2/c already at room temperature. Dielectric spectroscopy shows insulating behavior. Resonant inelastic x-ray scattering (RIXS) reveals a rich excitation spectrum below 1.5 eV with a sinusoidal dynamical structure factor that unambiguously demonstrates the quasi-molecular character of the electronic states. Below 0.3 eV, we observe a series of excitations. According to exact diagonalization calculations, such low-energy excitations reflect the proximity of Ba3InIr2O9 to a hopping-induced phase transition based on the condensation of a quasi-molecular spin-orbit exciton. The dimer ground state roughly hosts two holes in a bonding j=1/2 orbital and the third hole in a bonding j=3/2 orbital., Comment: 14 pages, 10 figures, V2: published version, minor changes

We present a comprehensive experimental and ab-initio study of the $S=1/2$ Mo$^{5+}$ system, KMoOP$_2$O$_7$, and show that it realizes the $S = 1/2$ Heisenberg chain antiferromagnet model. Powder neutron diffraction reveals that KMoOP$_2$O$_7$ forms a magnetic network comprised of pairs of Mo$^{5+}$ chains within its monoclinic $P2_1/n$ structure. Antiferromagnetic interactions within the Mo$^{5+}$ chains are identified through magnetometry measurements and confirmed by analysis of the magnetic specific heat. The latter reveals a broad feature centred on $T_\textrm{N} = 0.54$ K, which we ascribe to the onset of long-range antiferromagnetic order. No magnetic Bragg scattering is observed in powder neutron diffraction data collected at 0.05 K, however, which is consistent with a strongly suppressed ordered moment with an upper limit $\mu_\textrm{ord} < 0.15 \mu_\textrm{B}$. The one-dimensional character of the magnetic correlations in KMoOP$_2$O$_7$ is verified through analysis of inelastic neutron scattering data, resulting in a model with $J_\textrm{1} \approx 34$ K and $J_\textrm{2} \approx -2$ K for the intrachain and interchain exchange interactions, respectively. The origin of these experimental findings are addressed through density-functional theory calculations., Comment: 10 pages, 7 figures

We report the structural and magnetic properties of a new spin-$\frac12$ antiferromagnet NaZnVOPO$_4$(HPO$_4$) studied via x-ray diffraction, magnetic susceptibility, high-field magnetization, specific heat, and $^{31}$P nuclear magnetic resonance (NMR) measurements, as well as density-functional band-structure calculations. While thermodynamic properties of this compound are well described by the $J_1-J_2$ square-lattice model, \textit{ab initio} calculations suggest a significant deformation of the spin lattice. From fits to the magnetic susceptibility we determine the averaged nearest-neighbor and second-neighbor exchange couplings of $\bar J_1\simeq -1.3$ K and $\bar J_2\simeq 5.6$ K, respectively. Experimental saturation field of 15.3\,T is consistent with these estimates if 20\% spatial anisotropy in $J_1$ is taken into account. Specific heat data signal the onset of a magnetic long-range order at $T_{\rm N} \simeq 2.1$ K, which is further supported by a sharp peak in the NMR spin-lattice relaxation rate. The NMR spectra mark the superposition of two P lines due to two noneqivalent P sites where the broad line with the strong hyperfine coupling and short $T_1$ is identified as the P(1) site located within the magnetic planes, while the narrow line with the weak hyperfine coupling and long $T_1$ is designated as the P(2) site located between the planes., Comment: 13 pages, 11 figures

Crystal structure and thermodynamic properties of Na$_2$SrCo(PO$_4$)$_2$, the chemical sibling of the triangular quantum spin-liquid candidate Na$_2$BaCo(PO$_4$)$_2$, are reported. From single crystal x-ray diffraction and high-resolution synchrotron x-ray powder diffraction, the compound was found to crystallize in the monoclinic space group $P2_1/a$ at room temperature, in contrast to the trigonal Na$_2$BaCo(PO$_4$)$_2$. Above 650 K, the symmetry of Na$_2$SrCo(PO$_4$)$_2$ changes to $C2/m$, while around 1025 K a further transformation toward trigonal symmetry is observed. The monoclinic symmetry leads to a small deformation of the CoO$_6$ octahedra beyond the trigonal distortion ubiquitous in this structure type, and results in the stronger $g$-tensor anisotropy ($g_{\text{z}}/g_{\text{xy}} = 1.6 $) as well as the increased XXZ anisotropy ($J_{\text{z}}/J_{\text{xy}} = 2.1$) compared to the Ba compound ($g_{\text{z}}/g_{\text{xy}} = 1.1 $, $J_{\text{z}}/J_{\text{xy}} = 1.5$), while the average coupling strength, $J_{\text{av}}/k_{\text{B}}=(2J_{\text{xy}}+J_{\text{z}})/3k_\text{B}\simeq 1.3\,\text{K}$, remains unchanged. The N\'{e}el temperature increases from 140 mK (Ba) to 600 mK (Sr), and an uncompensated in-plane moment of $0.066(4)\mu_{\text{B}}/\text{f.u.}$ appears. We show that the ordering temperature of a triangular antiferromagnet is capably controlled by its structural distortions.

Geometric frustration inhibits magnetic systems from ordering, opening a window to unconventional phases of matter. The paradigmatic frustrated lattice in three dimensions to host a spin liquid is the pyrochlore, although there remain few experimental compounds thought to realize such a state. Here we go beyond the pyrochlore via molecular design in the metal-azolate framework [Mn(II)(ta)$_2$], which realizes a closely related centred pyrochlore lattice of Mn-spins with $S=5/2$. Despite a Curie-Weiss temperature of $-21$ K indicating the energy scale of magnetic interactions, [Mn(II)(ta)$_2$] orders at only 430 mK, putting it firmly in the category of highly frustrated magnets. Comparing magnetization and specific heat measurements to numerical results for a minimal Heisenberg model, we predict that this material displays distinct features of a classical spin liquid with a structure factor reflecting Coulomb physics in the presence of charges., Comment: Main: 6 pages, 3 figures. Supplementary: 15 pages, 12 figures. Updated Version

We study the crystal structure of the tetragonal iron selenide FeSe and its nematic phase transition to the low-temperature orthorhombic structure using synchrotron x-ray and neutron scattering analyzed in both real and reciprocal space. We show that in the local structure the orthorhombic distortion associated with the electronically driven nematic order is more pronounced at short length scales. It also survives up to temperatures above 90 K where reciprocal-space analysis suggests tetragonal symmetry. Additionally, the real-space pair distribution function analysis of the synchrotron x-ray diffraction data reveals a tiny broadening of the peaks corresponding to the nearest Fe-Fe, nearest Fe-Se, and the next-nearest Fe-Se bond distances as well as the tetrahedral torsion angles at a short length scale of 20 angstr\"om. This broadening appears below 20 K and is attributed to a pseudogap. However, we did not observe any further reduction in local symmetry below orthorhombic down to 3 K. Our results suggest that the superconducting gap anisotropy in FeSe is not associated with any symmetry-lowering short-range structural correlations., Comment: 9 pages, 6 figures

Antiferromagnetic and ferro/ferrimagnetic orders are typically exclusive in nature, thus, their co-existence in atomic-scale proximity is expected only in heterostructures. Breaking this paradigm and broadening the range of unconventional magnetic states, we report here on an atomic-scale hybrid spin state, which is stabilized in three-dimensional crystals of the polar antiferromagnet Co$_2$Mo$_3$O$_8$ by magnetic fields applied perpendicular to the \emph{Co} honeycomb layers and possesses a spontaneous in-plane ferromagnetic moment. Our microscopic spin model, capturing the observed field dependence of the longitudinal and transverse magnetization as well as the magnetoelectric/elastic properties, reveals that this novel spin state is composed of an alternating stacking of antiferromagnetic and ferrimagnetic honeycomb layers. The strong intra-layer and the weak inter-layer exchange couplings together with competing anisotropies at octahedral and tetrahedral \emph{Co} sites are identified as the key ingredients to stabilize antiferromagnetic and ferrimagnetic layers in such a close proximity. We show that the proper balance of magnetic interactions can extend the stability range of this hybrid phase down to zero magnetic field. The possibility to realize a layer-by-layer stacking of such distinct spin orders via suitable combinations of microscopic interactions opens a new dimension towards the nanoscale engineering of magnetic states.

Acoustic phonons have recently been posited as playing an integral role in explaining the half-quantized thermal Hall effect in $\alpha$-RuCl$_3$. Therefore, we present much needed inelastic x-ray scattering measurements of its acoustic phonon dispersion, along with calculations using the frozen-phonon method. We also discuss a temperature study which conclusively shows a first-order structural transition to a non-$C2/m$ space group at low temperature. Together these results are an important backbone for future theoretical and experimental studies of $\alpha$-RuCl$_3$.

Temperature-dependent reflectivity studies on the non-magnetic kagome metal RbV$_3$Sb$_5$ in a broad energy range (50 cm$^{-1}$ $-$ 20000 cm$^{-1}$, equivalent to 6 meV $-$ 2.5 eV) down to 10 K are reported. Below $T_{\rm CDW}=102$ K, the optical spectra demonstrate a prominent spectral-weight transfer from low to higher energies as the fingerprint of the charge-density wave (CDW) formation with the opening of a partial gap. A detailed analysis reveals two energy scales of, respectively, $\sim$ 800 cm$^{-1}$ (100 meV) and 360 cm$^{-1}$ (45 meV), the latter visible below 50 K only. Additionally, two modes at, respectively, 160 cm$^{-1}$ (20 meV) and 430 cm$^{-1}$ (53 meV) can be traced both above and below $T_{\rm CDW}$. They show strong anomalies already above $T_{\rm CDW}$ with a further renormalization across the transition, suggesting the importance of the electron-phonon coupling in RbV$_3$Sb$_5$ in both normal and CDW states. While the 160 cm$^{-1}$ mode can be attributed to the E$_{1u}$ phonon, the 430 cm$^{-1}$ mode could not be reproduced in our phonon calculations. The antiresonance nature of this mode suggests a nontrivial electron-phonon coupling in RbV$_3$Sb$_5$. A distinct localization peak observed at all temperatures signals damped electron dynamics, whereas the reduced Drude spectral weight manifests moderate deviations from the band picture in RbV$_3$Sb$_5$., Comment: 14 pages, 12 figures

We present magnetization measurements carried out on polycrystalline and single-crystalline samples of $\alpha$-Li$_2$IrO$_3$ under hydrostatic pressures up to 2 GPa and establish the temperature-pressure phase diagram of this material. The N\'eel temperature ($T_{\rm{N}}$) of $\alpha$-Li$_2$IrO$_3$ is slightly enhanced upon compression with $dT_{\rm{N}}/dp$ = 1.5 K/GPa. Above 1.2 GPa, $\alpha$-Li$_2$IrO$_3$ undergoes a first-order phase transition toward a nonmagnetic dimerized phase, with no traces of the magnetic phase observed above 1.8 GPa at low temperatures. The critical pressure of the structural dimerization is strongly temperature-dependent. This temperature dependence is well reproduced on the ab initio level by taking into account lower phonon entropy in the nonmagnetic phase. We further show that the initial increase in $T_{\rm{N}}$ of the magnetic phase is due to a weakening of the Kitaev interaction $K$ along with the enhancement of the Heisenberg term $J$ and off-diagonal anisotropy $\Gamma$. Our study reveals a common thread in the interplay of magnetism and dimerization in pressured Kitaev materials., Comment: 8 pages, 7 figures

We report on high-field electron spin resonance studies of two iridium hexahalide compounds, (NH$_4$)$_2$IrCl$_6$ and K$_2$IrCl$_6$. In the paramagnetic state, our measurements reveal isotropic $g$-factors $g = 1.79$(1) for the Ir$^{4+}$ ions, in agreement with their cubic symmetries. Most importantly, in the magnetically ordered state, we observe two magnon modes with zero-field gaps of 11.3 and 14.2 K for (NH$_4$)$_2$IrCl$_6$ and K$_2$IrCl$_6$, respectively. Based on that and using linear spin-wave theory, we estimate the nearest-neighbor exchange couplings and anisotropic Kitaev interactions, $J_1/k_B=10.3$ K, $K/k_B=0.7$ K for (NH$_4$)$_2$IrCl$_6$, and $J_1/k_B=13.8$ K, $K/k_B=0.9$ K for K$_2$IrCl$_6$, revealing the nearest-neighbor Heisenberg coupling as the leading interaction term, with only a weak Kitaev anisotropy.

Magnetism of the spin-$\frac12$ $\alpha$-KVOPO$_4$ is studied by thermodynamic measurements, $^{31}$P nuclear magnetic resonance (NMR), neutron diffraction, and density-functional band-structure calculations. Ferromagnetic Curie-Weiss temperature of $\theta_{\rm CW}\simeq 15.9$ K and the saturation field of $\mu_0H_s\simeq 11.3$ T suggest the predominant ferromagnetic coupling augmented by a weaker antiferromagnetic exchange that leads to a short-range order below 5 K and the long-range antiferromagnetic order below $T_{\rm N}\simeq 2.7$ K in zero field. Magnetic structure with the propagation vector $\mathbf k=(0,\frac12,0)$ and the ordered magnetic moment of 0.58 $\mu_B$ at 1.5 K exposes a non-trivial spin lattice where strong ferromagnetic dimers are coupled antiferromagnetically. The reduction in the ordered magnetic moment with respect to the classical value (1 $\mu_{\rm B}$) indicates sizable quantum fluctuations in this setting, despite the predominance of ferromagnetic exchange. We interpret this tendency toward ferromagnetism as arising from the effective orbital order in the folded chains of the VO$_6$ octahedra., Comment: 12 pages, 14 figures, 58 references

We present magnetization measurements on polycrystalline $\beta$-Li$_2$IrO$_3$ under hydrostatic pressures up to 3~GPa and construct the temperature-pressure phase diagram of this material. Our data confirm that magnetic order breaks down in a first-order phase transition at $p_{\rm{c}}$ $\approx$ 1.4~GPa and additionally reveal a step-like feature -- magnetic signature of structural dimerization -- that appears at $p_{\rm{c}}$ and shifts to higher temperatures upon further compression. Following the structural study by L. S. I. Veiga et al. [Phys. Rev. B 100, 064104 (2019)], we suggest that a partially dimerized phase with a mixture of magnetic and non-magnetic Ir$^{4+}$ sites develops above $p_{\rm{c}}$. This phase is thermodynamically stable between 1.7 and 2.7~GPa according to our ab initio calculations. It confines the magnetic Ir$^{4+}$ sites to weakly coupled tetramers with a singlet ground state and no long-range magnetic order. Our results rule out the formation of a pressure-induced spin-liquid phase in $\beta$-Li$_2$IrO$_3$ and reveal peculiarities of the magnetism collapse transition in a Kitaev material. We also show that a compressive strain imposed by the pressure treatment of $\beta$-Li$_2$IrO$_3$ enhances signatures of the 100~K magnetic anomaly at ambient pressure., Comment: 10 pages, 10 figures

We report the crystal structure and magnetic behavior of the $4d^3$ spin-$\frac32$ silicophosphate MoP$_3$SiO$_{11}$ studied by high-resolution synchrotron x-ray diffraction, neutron diffraction, thermodynamic measurements, and ab initio band-structure calculations. Our data revise the crystallographic symmetry of this compound and establish its rhombohedral space group ($R\bar 3c$) along with the geometrically perfect honeycomb lattice of the Mo$^{3+}$ ions residing in disconnected MoO$_6$ octahedra. Long-range antiferromagnetic order with the propagation vector $\mathbf k=0$ observed below $T_N=6.8$ K is a combined effect of the nearest-neighbor in-plane exchange coupling $J\simeq 2.6$ K, easy-plane single-ion anisotropy $D\simeq 2.2 $ K, and a weak interlayer coupling $J_c\simeq 0.8$ K. The 12% reduction in the ordered magnetic moment of the Mo$^{3+}$ ions and the magnon gap of $\Delta\simeq 7$ K induced by the single-ion anisotropy further illustrate the impact of spin-orbit coupling on the magnetism. Our analysis puts forward single-ion anisotropy as an important ingredient of $4d^3$ honeycomb antiferromagnets despite their nominally quenched orbital moment., Comment: published version

A single ferromagnetic kagome layer is predicted to realize a Chern insulator with quantized Hall conductance, which upon stacking can become a Weyl-semimetal with large anomalous Hall effect (AHE) and magneto-optical activity. Indeed, in the kagome bilayer material Fe$_3$Sn$_2$, a large AHE was detected, however, it still awaits the direct probing of the responsible band structure features by bulk sensitive methods. We measure the optical, both diagonal and Hall, conductivity spectra over a broad spectral range and identify the origin of the intrinsic AHE with the help of momentum- and band-decomposed first-principles calculations. We find that low-energy transitions, tracing "helical volumes" in momentum space reminiscent of the formerly predicted helical nodal lines, substantially contribute to the AHE, which is further increased by contributions from multiple higher-energy interband transitions. Our study also reveals that local Coulomb interactions lead to band reconstructions near the Fermi level.

We report x-ray diffraction, magnetic susceptibility, heat capacity, $^{1}$H nuclear magnetic resonance (NMR), and muon spin relaxation ($\mu$SR) measurements, as well as density-functional band-structure calculations for the frustrated $S=3/2$ triangular lattice Heisenberg antiferromagnet (TLHAF) $\alpha$-HCrO$_{2}$ (trigonal, space group: $R\bar{3}m$). This compound undergoes a clear magnetic transition at $T_{\rm N} \simeq 22.5$~K, as seen from the drop in the muon paramagnetic fraction and concurrent anomalies in the magnetic susceptibility and specific heat. Local probes (NMR and $\mu$SR) reveal a broad regime with slow fluctuations down to $0.7\,T_{\rm N}$, this temperature corresponding to the maximum in the $\mu$SR relaxation rate and in the NMR wipe-out. From the comparison with NaCrO$_{2}$ and $\alpha$-KCrO$_{2}$, the fluctuating regime and slow dynamics below $T_{\rm N}$ appear to be hallmarks of the TLHAF with $ABC$ stacking that leads to a frustration of interlayer couplings between the triangular planes. This interlayer frustration is a powerful lever to generate spin states with persistent dynamics and may bear implications to spin-liquid candidates with the triangular geometry., Comment: 14 pages, 11 figures, 2 tables

Temperature-dependent reflectivity measurements on the kagome metal CsV$_3$Sb$_5$ in a broad frequency range of $50-20000$ cm$^{-1}$ down to $T$=10 K are reported. The charge-density wave (CDW) formed below $T_{\rm CDW}$ = 94 K manifests itself in a prominent spectral-weight transfer from low to higher energy regions. The CDW gap of 60-75 meV is observed at the lowest temperature and shows significant deviations from an isotropic BCS-type mean-field behavior. Absorption peaks appear at frequencies as low as 200 cm$^{-1}$ and can be identified with interband transitions according to density-functional calculations. The change in the interband absorption compared to KV$_3$Sb$_5$ reflects the inversion of band saddle points between the K and Cs compounds. Additionally, a broader and strongly temperature-dependent absorption feature is observed below 1000 cm$^{-1}$ and assigned to a displaced Drude peak. It reflects localization effects on charge carriers., Comment: 9 pages, 7 figures

Coexisting density-wave and superconducting states along with the large anomalous Hall effect in the absence of local magnetism remain intriguing and enigmatic features of the AV$_3$Sb$_5$ kagome metals (A = K, Rb, Cs). Here, we demonstrate via optical spectroscopy and density-functional calculations that low-energy dynamics of KV$_3$Sb$_5$ is characterized by unconventional localized carriers, which are strongly renormalized across the density-wave transition and indicative of electronic correlations. Strong phonon anomalies are prominent not only below the density-wave transition, but also at high temperatures, suggesting an intricate interplay of phonons with the underlying electronic structure. We further propose the star-of-David and tri-hexagon (inverse star-of-David) configurations for the density-wave order in KV$_3$Sb$_5$. These configurations are strongly reminiscent of $p$-wave states expected in the Hubbard model on the kagome lattice at the filling level of the van Hove singularity. The proximity to this regime should have intriguing and far-reaching implications for the physics of KV$_3$Sb$_5$ and related materials., Comment: Main text + Supplementary

Li$_2$Sr[MnN]$_2$ single crystals were successfully grown out of Li rich flux. The crystal structure was determined by single crystal X-ray diffraction and revealed almost linear $-$N$-$Mn$-$N$-$Mn$-$ chains as central structural motif. Tetragonal columns of this air and moisture sensitive nitridomanganate were employed for electrical transport, heat capacity, and anisotropic magnetization measurements. Both the electronic and magnetic properties are most remarkable, in particular the linear increase of the magnetic susceptibility with temperature that is reminiscent of underdoped cuprate and Fe-based superconductors. Clear indications for antiferromagnetic ordering at $T_{\rm N} = 290$ K were obtained. Metallic transport behavior is experimentally observed in accordance with electronic band structure calculations., Comment: 12 pages, 7 figures

Generation of very low temperatures has been crucially important for applications and fundamental research, as low-temperature quantum coherence enables operation of quantum computers and formation of exotic quantum states, such as superfluidity and superconductivity. One of the major techniques to reach milli-Kelvin temperatures is adiabatic demagnetization refrigeration (ADR). This method uses almost non-interacting magnetic moments of paramagnetic salts where large distances suppress interactions between the magnetic ions. The large spatial separations are facilitated by water molecules, with a drawback of reduced stability of the material. Here, we show that an H$_2$O-free frustrated magnet KBaYb(BO$_3$)$_2$ can be ideal refrigerant for ADR, achieving at least 22\,mK upon demagnetization under adiabatic conditions. Compared to conventional refrigerants, KBaYb(BO$_3)_2$ does not degrade even under high temperatures and ultra-high vacuum conditions. Further, its frustrated magnetic network and structural randomness enable cooling to temperatures several times lower than the energy scale of magnetic interactions, which is the main limiting factor for the base temperature of conventional refrigerants., Comment: accepted for publication in Communications Materials