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The magnetic insulator Nd$_3$BWO$_9$ has been proposed as a proximate spin-liquid candidate, realizing the highly frustrated breathing kagome lattice. We report a combination of single-crystal neutron scattering studies and numerical simulations, showing that it is the inter-plane couplings that determine the physics. To explain the exotic magnetism, we derive a simple one-dimensional Ising model composed of twisted triangular spin-tubes, i.e., triple braids of Ising spin chains with almost-orthogonal anisotropy frames and competing ferro-antiferromagnetic interactions. This model can account for the ground state, excitations, the numerous field-induced fractional magnetization plateau phases and incommensurate magnetic correlations at elevated temperatures., Comment: 6 pages, 4 figures (SM 7 pages, 6 figures)

The magnetic properties of Ho-doped langasites (La:Ho)$_3$Ga$_5$SiO$_{14}$ are dominated by the Ising-like magnetic moments of the Ho$^{3+}$ ions. In their saturated regime, the induced magnetic state breaks both time and space inversion symmetries, leading to a novel linear magnetoelectric effect. However, due to distortions induced by a shared Ga/Si occupancy of the 2d sites, resolving the microscopic nature of the magnetic configuration remains a difficult task. Here we combine polarized neutron diffraction and angular dependent magnetization experiments to determine the local distortions of the Ho$^{3+}$ magnetic moments in doped langasites (La$_{1-x}$Ho$_x$)$_3$Ga$_5$SiO$_{14}$ with $x \approx 0.015$ and $x \approx 0.045$. We propose a model for a field-induced magnetic configuration with arbitrary orientations of the local Ising axis of Ho$^{3+}$ in distorted positions. The operations of broken local $C_2$ symmetry and rotations around the trigonal $C_3$ axis connect different sites, restoring the global P321 symmetry of the crystal and simplifying the description of the magnetic properties. The superposition of two distorted Ho$^{3+}$ positions connected by $C_2$ symmetry determines the local magnetic susceptibility tensor, which no longer appears Ising-like at low fields.

The antiferromagnetic structure of Yb$_{3}$Ga$_{5}$O$_{12}$ is identified by neutron diffraction experiments below the previously-known transition at $T_{\lambda}=54$ mK. The magnetic propagation vector is found to be ${\bf k}=(1/2, 1/2, 0)$, an unusual wave-vector in the garnet structure. The associated complex magnetic structure highlights the role of exchange interactions in a nearly isotropic system dominated by dipolar interactions and finds echos with exotic structures theoretically proposed. Reduced values of the ordered moments may indicate significant quantum fluctuations in this effective spin-1/2 geometrically frustrated magnet.

Magnetic structures and spin excitations are studied across the phase diagram of the geometrically frustrated S = 3/2 quantum antiferromagnet Cs2CoBr4 in magnetic fields applied along the magnetic easy axis, using neutron diffraction, inelastic neutron scattering and THz absorption spectroscopy. The data are analyzed, where appropriate, using extended SU (4) linear spin wave theory. A minimal magnetic Hamiltonian is proposed based on measurements in the high field polarized state. It deviates considerably from the previously considered models. Additional dilatometry experiments highlight the importance of magnetoelastic coupling in this system., Comment: 14 pages, 10 figures, Accepted to Phys. Rev. B

The discovery of multiple superconducting phases in UTe2 boosted research on correlated-electron physics. This heavy-fermion paramagnet was rapidly identified as a reference compound to study the interplay between magnetism and unconventional superconductivity with multiple degrees of freedom. The proximity to a ferromagnetic quantum phase transition was initially proposed as a driving force to triplet-pairing superconductivity. However, we find here that long-range incommensurate antiferromagnetic order is established under pressure. The propagation vector km = (0.07,0.33,1) of the antiferromagnetic phase is close to a wavevector where antiferromagnetic fluctuations have previously been observed at ambient pressure. These elements support that UTe2 is a nearly-antiferromagnet at ambient pressure. Our work appeals for theories modelling the evolution of the magnetic interactions and electronic properties, driving a correlated paramagnetic regime at ambient pressure to a long-range antiferromagnetic order under pressure. A deeper understanding of itinerant-f-electrons magnetism in UTe2 will be a key for describing its unconventional superconducting phases., Comment: Article: 17 pages, 4 figures, 64 references Supplementary Information: 6 pages, 6 figures, 7 references

Y3Cu9(OH)19Cl8 realizes an original anisotropic kagome model hosting a rich magnetic phase diagram [M. Hering et al, npj Computational Materials 8, 1 (2022)]. We present an improved synthesis of large phase-pure single crystals via an external gradient method. These crystals were investigated in details by susceptibility, specific heat, thermal expansion, neutron scattering and local muSR and NMR techniques. At variance with polycristalline samples, the study of single crystals gives evidence for subtle structural instabilities at 33K and 13K which preserve the global symmetry of the system and thus the magnetic model. At 2.1K the compound shows a magnetic transition to a coplanar (1/3,1/3) long range order as predicted theoretically. However our analysis of the spin wave excitations yields magnetic interactions which locate the compound closer to the phase boundary to a classical jammed spin liquid phase. Enhanced quantum fluctuations at this boundary may be responsible for the strongly reduced ordered moment of the Cu2+, estimated to be 0.075muB from muSR.

We present a single-crystal neutron diffraction study on the Shastry-Sutherland lattice system TbB$_4$ at zero magnetic field and under pulsed high magnetic fields up to 35 T applied along the crystallographic $c$ axis. While our results confirm the magnetic structures at zero-field as well as those at the half- and full-magnetization plateaus, they offer new insight into the $\frac{2}{9}$- and $\frac{1}{3}$-magnetization plateaus observed in this system. A stripe model of polarized 4-spin-plaquettes whose stripe density proportionally increases with the macroscopic magnetization is in full agreement with the neutron diffraction data. Equally well suited alternative models exist which explain the observed Bragg peaks which are inherently limited in a pulsed high magnetic field experiment. We discuss the different intensity distribution in $Q$ space which can be used to distinguish these models in future experiments.

We report a comprehensive experimental investigation of the magnetic structure of the cycloidal phase in Ca$_3$Ru$_2$O$_7$, which mediates the spin reorientation transition, and establishes its magnetic phase diagram. In zero applied field, single-crystal neutron diffraction data confirms the scenario deduced from an earlier resonant x-ray scattering study: between $46.7$~K $< T < 49.0$~K the magnetic moments form a cycloid in the $a-b$ plane with a propagation wavevector of $(\delta,0,1)$ with $\delta \simeq 0.025$ and an ordered moment of about 1 $\mu_{\rm{B}}$, with the eccentricity of the cycloid evolving with temperature. In an applied magnetic field applied parallel to the $b$-axis, the intensity of the $(\delta,0,1)$ satellite peaks decreases continuously up to about $\mu_0 H \simeq 5$ T, above which field the system becomes field polarised. Both the eccentricity of the cycloid and the wavevector increase with field, the latter suggesting an enhancement of the anti$-$symmetric Dzyaloshinskii$-$Moriya interaction via magnetostriction effects. Transitions between the various low-temperature magnetic phases have been carefully mapped out using magnetometry and resistivity. The resulting phase diagram reveals that the cycloid phase exists in a temperature window that expands rapidly with increasing field, before transitioning to a polarised paramagnetic state at 5 T. High-field magnetoresistance measurements show that below $T\simeq 70$ K the resistivity increases continuously with decreasing temperature, indicating the inherent insulating nature at low temperatures of our high-quality, untwinned, single-crystals. We discuss our results with reference to previous reports of the magnetic phase diagram of Ca$_3$Ru$_2$O$_7$ that utilised samples which were more metallic and/or poly-domain., Comment: 12 pages, 11 figures

We theoretically and experimentally study the stability of the unconventional fractional antiferromagnetic skyrmion lattice (AF-SkL) in Mn$_2$S$_4$ spinel under magnetic fields applied along the $[$1-10$]$ crystal direction. By performing numerical Monte Carlo simulations for the minimal effective spin model that we proposed in Ref. [S. Gao, et al., Nature 586, 37-41 (2020)], we show that the skyrmion lattice is aligned within the equivalent and symmetric $[$1-11$]$ or $[$1-11$]$ planes, which are equally inclined to the applied magnetic field. We attribute this behavior to the magnetic anisotropy of the host material. Neutron single crystal diffraction presents a very good agreement with the predictions of the effective model. It reveals that the topological spin texture gets destabilized at low temperatures and moderate magnetic fields and is replaced by a conical phase for B// $[$1-10$]$. The present study elucidates the central role of the magnetic anisotropy in the stabilization of antiferromagnetic skyrmionic states., Comment: Accepted in PRB

We report an excellent realization of the highly non-classical incommensurate spin-density wave (SDW) state in the quantum frustrated antiferromagnetic insulator Cs$_2$CoBr$_4$. In contrast to the well-known Ising spin chain case, here the SDW is stabilized by virtue of competing planar in-chain anisotropies and frustrated interchain exchange. Adjacent to the SDW phase is a broad $m = 1/3$ magnetization plateau that can be seen as a commensurate locking of the SDW state into the up-up-down (UUD) spin structure. This represents the first example of long-sought SDW-UUD transition in triangular-type quantum magnets., Comment: 13 pages, 13 figures

Single crystal elastic and inelastic neutron scattering experiments are performed on the frustrated ferro-antiferromagnet SrZnVO(PO4)2 in high magnetic fields. The fully polarized state, the presaturation phase and the columnar-antiferromagnetic phase just bellow the presaturation phase were investigated. The observed renormalization of spin wave bandwidths, re-distribution of intensities between different branches and non-linearities in the magnetization curve are all indicative of strong deviations from classical spin wave theory. The previously observed presaturation transition is attributed to a staggered pattern of Dzyaloshinskii-Moriya interactions., Comment: Changes: author list in meta data corrected

We report a neutron diffraction study of single-crystal CePtAl$_3$ complemented by measurements of the specific heat under applied magnetic field. Below $T_\mathrm{N}$=3 K CePtAl$_3$ develops incommensurate antiferromagnetic order with a single modulation vector $\vec{k}$=$(0.676 \, 0 \, 0)$. Residual magnetic scattering intensity above $T_\mathrm{N}$ and a broadening of the specific heat anomaly at $T_\mathrm{N}$ may be consistently described in terms of a Gaussian distribution of transition temperatures with a standard deviation $\sigma\approx0.5\,{\rm K}$. The distribution of $T_\mathrm{N}$ may be attributed to the observation of occupational and positional disorder between the Pt and Al sites. Measurements under magnetic field reveal unusual changes of the domain populations when the field is applied along the $[0\,1\,0]$ direction consistent with a transition from cycloidal to amplitude modulated magnetic order around 2.5 T., Comment: v1: Draft on CePtAl3 and CePdAl3. Later split into separate papers regarding each compound separately. v2: Before submission. Major reworks from v1. v3: Final. After peer review and proofs

We investigate ytterbium gallium garnet Yb$_{3}$Ga$_{5}$O$_{12}$ in the paramagnetic phase above the supposed magnetic transition at $T_{\lambda} \approx 54$ mK. Our study combines susceptibility and specific heat measurements with neutron scattering experiments and theoretical calculations. Below 500 mK, the elastic neutron response is strongly peaked in the momentum space. Along with that the inelastic spectrum develops flat excitation modes. In magnetic field, the lowest energy branch follows a Zeeman shift in accordance with the field-dependent specific heat data. An intermediate state with spin canting away from the field direction is evidenced in small magnetic fields. In the field of 2 T, the total magnetization almost saturates and the measured excitation spectrum is well reproduced by the spin-wave calculations taking into account solely the dipole-dipole interactions. The small positive Curie-Weiss temperature derived from the susceptibility measurements is also accounted for by the dipole spin model. Altogether, our results suggest that Yb$_{3}$Ga$_{5}$O$_{12}$ is a quantum dipolar magnet., Comment: 12 pages, 10 figures

By combining neutron scattering and magnetization measurements down to 80 mK, we determine the $(H,T)$ phase diagram of the Nd$_2$(Zr$_{1-x}$Ti$_x$)$_2$O$_7$ pyrochlore magnet compounds. In those samples, Zr is partially substituted by Ti, hence tuning the exchange parameters and testing the robustness of the various phases. In all samples, the ground state remains "all in / all out", while the field induces phase transitions towards new states characterized by "2 in - 2 out" or "1 out - 3 in / 1 in - 3 out" configurations. These transitions manifest as metamagnetic singularities in the magnetization vs field measurements. Strikingly, it is found that moderate substitution reinforces the stability of the "all in / all out" phase: the N\'eel temperature, the metamagnetic fields along with the ordered magnetic moment are higher in substituted samples with $x <$ 10\%., Comment: 14 pages, 17 figures + appendices

Magnetic and crystallographic transitions in the Cairo pentagonal magnet Bi2Fe4O9 are investigated by means of infrared synchrotron-based spectroscopy as a function of temperature (20 - 300 K) and pressure (0 - 15.5 GPa). One of the phonon modes is shown to exhibit an anomalous softening as a function of temperature in the antiferromagnetic phase below 240 K, highlighting spin-lattice coupling. Moreover, under applied pressure at 40 K, an even larger softening is observed through the pressure induced structural transition. Lattice dynamical calculations reveal that this mode is indeed very peculiar as it involves a minimal bending of the strongest superexchange path in the pentagonal planes, as well as a decrease of the distances between second neighbor irons. The latter confirms the hypothesis made by Friedrich et al.,1 about an increase in the oxygen coordination of irons being at the origin of the pressure-induced structural transition. As a consequence, one expects a new magnetic superexchange path that may alter the magnetic structure under pressure., Comment: 11 pages, 8 figures, 5 tables

We investigate the temperature dependence of the spin dynamics in the pyrochlore magnet Nd$_2$Zr$_2$O$_7$ by neutron scattering experiments. At low temperature, this material undergoes a transition towards an "all in - all out" antiferromagnetic phase and the spin dynamics encompass a dispersion-less mode, characterized by a dynamical spin ice structure factor. Unexpectedly, this mode is found to survive above $T_{\rm N} \approx 300$ mK. Concomitantly, elastic correlations of the spin ice type develop. These are the signatures of a peculiar correlated paramagnetic phase which can be considered as a new example of Coulomb phase. Our observations near $T_{\rm N}$ do not reproduce the signatures expected for a Higgs transition, but show reminiscent features of the "all in - all out" order superimposed on a Coulomb phase., Comment: 6 pages + 9 pages supp. mat

The research field of magnetic frustration is dominated by triangle-based lattices but exotic phenomena can also be observed in pentagonal networks. A peculiar noncollinear magnetic order is indeed known to be stabilized in Bi2Fe4O9 materializing a Cairo pentagonal lattice. We present the spin wave excitations in the magnetically ordered state, obtained by inelastic neutron scattering. They reveal an unconventional excited state related to local precession of pairs of spins. The magnetic excitations are then modeled to determine the superexchange interactions for which the frustration is indeed at the origin of the spin arrangement. This analysis unveils a hierarchy in the interactions, leading to a paramagnetic state (close to the N\'eel temperature) constituted of strongly coupled dimers separated by much less correlated spins. This produces two types of response to an applied magnetic field associated with the two nonequivalent Fe sites, as observed in the magnetization distributions obtained using polarized neutrons., Comment: Article: 6 pages, 3 figures. Supplemental Material: 10 pages, 10 figures

Magnetization, magnetocaloric, calorimetric, neutron and X-ray diffraction and inelastic neutron scattering measurements are performed on single crystals of BaCdVO(PO$_4$)$_2$. The low-temperature crystal structure is found to be of a lower symmetry than previously assumed. The result is a more complicated model spin Hamiltonian, which we infer from measurements of the spin wave dispersion spectrum. The main finding is a novel spin state which emerges in high magnetic fields after antiferromagnetic order is terminated at $H_{c1}\simeq 4.0$ T. It is a distinct thermodynamic phase with a well-defined phase boundary at $H_{c2}\simeq 6.5$ T and is clearly separate from the fully saturated phase. Yet, it shows no conventional (dipolar) magnetic long range order. We argue that it is fully consistent with the expectations for a quantum bond-nematic state.

The notion of a simple ordered state implies homogeneity. If the order is established by a broken symmetry, elementary Landau theory of phase transitions shows that only one symmetry mode describes this state. Precisely at points of phase coexistence domain states formed of large regions of different phases can be stabilized by long range interactions. In uniaxial antiferromagnets the so-called metamagnetism is an example of such a behavior, when an antiferromagnetic and field-induced spin-polarized paramagnetic/ferromagnetic state co-exist at a jump-like transition in the magnetic phase diagram. Here, combining experiment with theoretical analysis, we show that a different type of mixed state between antiferromagnetism and ferromagnetism can be created in certain acentric materials. In the small-angle neutron scattering experiments we observe a field-driven spin-state in the layered antiferromagnet Ca3Ru2O7, which is modulated on a scale between 8 and 20 nm and has both antiferromagnetic and ferromagnetic parts. We call this state a metamagnetic texture and explain its appearance by the chiral twisting effects of the asymmetric Dzyaloshinskii-Moriya (DM) exchange. The observation can be understood as an extraordinary coexistence, in one thermodynamic state, of spin orders belonging to different symmetries. Experimentally, the complex nature of this metamagnetic state is demonstrated by measurements of anomalies in electronic transport which reflect the spin-polarization in the metamagnetic texture, determination of the magnetic orbital moments, which supports the existence of strong spin-orbit effects, a pre-requisite for the mechanism of twisted magnetic states in this material., Comment: Supplementary materials included

We report the direct observation of a magnetic-feld induced long-wavelength spin spiral modulation in the chiral compound Ba3TaFe3Si2O14. This new spin texture emerges out of a chiral helical ground state, and is hallmarked by the onset of a unique contribution to the bulk electric polarization, the sign of which depends on the crystal chirality. The periodicity of the feld induced modulation, several hundreds of nm depending on the field value, is comparable to the length scales of mesoscopic topological defects such as skyrmions, merons and solitons. The phase transition and observed threshold behavior are consistent with a phenomenology based on the allowed Lifshitz invariants for the chiral symmetry of langasite, which intriguingly contain all the ingredients for the possible realization of topologically stable antiferromagnetic skyrmions.

We report single-crystal neutron diffraction study of the magnetic structure of the multiferroic compound YbMnO$_3$, a member of the hexagonal manganite family, in zero-field and under a magnetic field applied along the $c$-axis. We propose a scenario for the zero-field magnetic ordering and for the field-induced magnetic reorientation of the Mn and of the two Yb on distinct crystallographic sites, compatible with the macroscopic measurements, as well as with previous powder neutron diffraction experiment and results from other techniques (optical second harmonic generation, M\"ossbauer spectroscopy). Our study should contribute in settling some debated issues about the magnetic properties of this material, as part of a broader investigation of the entire hexagonal RMnO$_3$ (R = Dy, Ho, Er, Tm, Yb, Lu, Y) family.

The field induced quantum phase transitions in the disorder-free and disordered samples of the spin ladder material (CH_3)_2CHNH_3Cu(Cl_{1-x}Br_x)_3 are studied using magnetic calorimetry and magnetic neutron diffraction on single crystal samples. Drastically different critical indexes and correlation lengths in the high field phase are found for two different orientations of the applied field. It is argued that for a field applied along the crystallographic c axis, as in previous studies [1], the transition is best described as an Ising transition in random field and anisotropy, rather than as a magnetic Bose Glass to Bose Condensate transition. [1] Tao Hong, A. Zheludev, H. Manaka, and L.- P. Regnault, Phys. Rev. B 81, 060410 (2010).

The search for two dimensional quantum spin liquids, exotic magnetic states with an entangled ground state remaining disordered down to zero temperature, has been a great challenge in frustrated magnetism during the last decades. Recently, fractionalized excitations, called spinons, emerging from these states, have been evidenced in kagome and triangular antiferromagnets. In contrast, quantum ferromagnetic spin liquids in two dimensions, namely quantum kagome ices, have been less investigated, yet their classical counterparts exhibit amazing properties, magnetic monopole crystals as well as magnetic fragmentation. Here we show that, by applying a magnetic field on the pyrochlore oxide Nd$_2$Zr$_2$O$_7$, which has been shown to develop three dimensional quantum magnetic fragmentation in zero field, we are able to reduce the dimension of the system and to create a dynamic kagome ice state. Our results open the way to the observation of the quantum kagome ice state which was recently investigated theoretically., Comment: 7 pages, 4 figures + Supplementary information

Antiferromagnetic hexagonal MnTe is a promising material for spintronic devices relying on the control of antiferromagnetic domain orientations. Here we report on neutron diffraction, magnetotransport, and magnetometry experiments on semiconducting epitaxial MnTe thin films together with density functional theory (DFT) calculations of the magnetic anisotropies. The easy axes of the magnetic moments within the hexagonal basal plane are determined to be along $\left<1\bar100\right>$ directions. The spin-flop transition and concomitant repopulation of domains in strong magnetic fields is observed. Using epitaxially induced strain the onset of the spin-flop transition changes from $\sim2$~T to $\sim0.5$~T for films grown on InP and SrF$_2$ substrates, respectively., Comment: 9 pages, 7 figures

Nd0.05Ce0.95CoIn5 features a magnetic field-driven quantum phase transition that separates two antiferromagnetic phases with an identical magnetic structure inside the superconducting condensate. Using neutron diffraction we demonstrate that the population of the two magnetic domains in the two phases is affected differently by the rotation of the magnetic field in the tetragonal basal plane. In the low-field SDW-phase the domain population is only weakly affected while in the high-field Q-phase they undergo a sharp switch for fields around the a-axis. Our results provide evidence that the anisotropic spin susceptibility in both phases arises ultimately from spin-orbit interactions but are qualitatively different in the two phases. This provides evidence that the electronic structure is changed at the quantum phase transition, which yields a modified coupling between magnetism and superconductivity in the Q-phase.

The magnetic properties and magnetic structure are presented for CoPS$_3$, a quasi-two-dimensional antiferromagnet on a honeycomb lattice with a N\'eel temperature of $T_N \sim 120$ K. The compound is shown to have XY-like anisotropy in its susceptibility, and the anisotropy is analysed to extract crystal field parameters. For temperatures between 2 K and 300 K, no phase transitions were observed in the field-dependent magnetization up to 10 Tesla. Single-crystal neutron diffraction shows that the magnetic propagation vector is {\bf{k}}= $\left[010\right]$ with the moments mostly along the $\mathbf{a}$ axis and with a small component along the $\mathbf{c}$ axis, which largely verifies the previously-published magnetic structure for this compound. The magnetic Bragg peak intensity decreases with increasing temperature as a power law with exponent $2\beta = 0.60 \pm 0.01$ for $T > 0.9~T_N$., Comment: 24 pages, 8 figures

We report magnetic and thermodynamic properties of a $4d^1$ (Mo$^{5+}$) magnetic insulator MoOPO$_4$ single crystal, which realizes a $J_1$-$J_2$ Heisenberg spin-$1/2$ model on a stacked square lattice. The specific-heat measurements show a magnetic transition at 16 K which is also confirmed by magnetic susceptibility, ESR, and neutron diffraction measurements. Magnetic entropy deduced from the specific heat corresponds to a two-level degree of freedom per Mo$^{5+}$ ion, and the effective moment from the susceptibility corresponds to the spin-only value. Using {\it ab initio} quantum chemistry calculations we demonstrate that the Mo$^{5+}$ ion hosts a purely spin-$1/2$ magnetic moment, indicating negligible effects of spin-orbit interaction. The quenched orbital moments originate from the large displacement of Mo ions inside the MoO$_6$ octahedra along the apical direction. The ground state is shown by neutron diffraction to support a collinear N\'eel-type magnetic order, and a spin-flop transition is observed around an applied magnetic field of 3.5 T. The magnetic phase diagram is reproduced by a mean-field calculation assuming a small easy-axis anisotropy in the exchange interactions. Our results suggest $4d$ molybdates as an alternative playground to search for model quantum magnets., Comment: 9 pages, 7 figures

We compare theoretical results for electron spin resonance (ESR) properties of the Heisenberg-Ising Hamiltonian with ESR experiments on the quasi-one-dimensional magnet Cu(py)$_2$Br$_2$ (CPB). Our measurements were performed over a wide frequency and temperature range giving insight into spin dynamics, spin structure, and magnetic anisotropy of this compound. By analyzing the angular dependence of ESR parameters (resonance shift and linewidth) at room temperature we show that the two weakly coupled inequivalent spin chain types inside the compound are well described by Heisenberg-Ising chains with their magnetic anisotropy axes perpendicular to the chain direction and almost perpendicular to each other. We further determine the full $g$-tensor from these data. In addition, the angular dependence of the linewidth at high temperatures gives us access to the exponent of the algebraic decay of a dynamical correlation function of the isotropic Heisenberg chain. From the temperature dependence of static susceptibilities we extract the strength of the exchange coupling ($J/k_B = 52.0\,\text{K}$) and the anisotropy parameter ($\delta\approx -0.02$) of the model Hamiltonian. An independent compatible value of $\delta$ is obtained by comparing the exact prediction for the resonance shift at low temperatures with high-frequency ESR data recorded at $4\,\text{K}$. The spin structure in the ordered state implied by the two (almost) perpendicular anisotropy axes is in accordance with the propagation vector determined from neutron scattering experiments. In addition to undoped samples we study the impact of partial substitution of Br by Cl ions on spin dynamics. From the dependence of the ESR linewidth on doping level we infer an effective decoupling of the anisotropic component $J\delta$ from the isotropic exchange $J$ in these systems., Comment: 26 pages, 12 figures, section V.A.2 revised, appendices A and B shortened

We report a single-crystal neutron diffraction and inelastic neutron scattering study on the spin 1/2 cuprate Cu$_3$Bi(SeO$_3$)$_2$O$_2$Cl, complemented by dielectric and electric polarization measurements. The study clarifies a number of open issues concerning this complex material, whose frustrated interactions on a kagome-like lattice, combined with Dzyaloshinskii-Moriya interactions, are expected to stabilize an exotic canted antiferromagnetic order. In particular, we determine the nature of the structural transition occurring at 115 K, the magnetic structure below 25 K resolved in the updated space group, and the microscopic ingredients at the origin of this magnetic arrangement. This was achieved by an analysis of the measured gapped spin waves, which signifies the need of an unexpected and significant anisotropic exchange beyond the proposed Dzyaloshinskii-Moriya interactions. Finally, we discuss the mutliferroic properties of this material with respect to the space group symmetries.

The magnetic structure of the heavy fermion antiferromagnet CePt$_2$In$_7$ is determined using neutron diffraction. We find a magnetic wave vector $\mathbf{q}_M = (1/2,1/2,1/2)$, which is temperature independent up to $T_N =$ 5.5 K. A staggered moment of 0.45(1)$\mu_B$ at 2 K resides on the Ce ion. The nearest-neighbor moments in the tetragonal basal plane are aligned antiferromagnetically. The moments rotate by 90$^\circ$ from one CeIn$_3$ plane to another along the $c$ axis. A much weaker satellite peak with an incommensurate magnetic wave vector $\mathbf{q}_M = (1/2,1/2,0.47)$ seems to develop at low temperature. However, the experimental data available so far are not sufficient to draw a definitive conclusion about the possible co-existence of commensurate and incommensurate magnetic structures in this material., Comment: accepted for publication in Phys. Rev. B Rapid. Comm

We explore the field-temperature phase diagram of the XY pyrochlore antiferromagnet Er$_2$Ti$_2$O$_7$, by means of magnetization and neutron diffraction experiments. Depending on the field strength and direction relative to the high symmetry cubic directions $[001], [1\bar{1}0]$ and $[111]$, the refined field induced magnetic structures are derived from the zero field $\psi_2$ and $\psi_3$ states of the $\Gamma_5$ irreducible representation which describes the ground state of XY pyrochlore antiferromagnets. At low field, domain selection effects are systematically at play. In addition, for $[001]$, a phase transition is reported towards a $\psi_3$ structure at a characteristic field $H_c^{001}=$ 43 mT. For $[1\bar{1}0]$ and $[111]$, the spins are continuously tilted by the field from the $\psi_2$ state, and no phase transition is found while domain selection gives rise to sharp anomalies in the field dependence of the Bragg peaks intensity. For $[1\bar{1}0]$, these results are confirmed by high resolution inelastic neutron scattering experiments, which in addition allow us to determine the field dependence of the spin gap. This study agrees qualitatively with the scenario proposed theoretically by Maryasin {\it et al.} [Phys. Rev. B {\bf 93}, 100406(R) (2016)], yet the strength of the field induced anisotropies is significantly different from theory., Comment: 14 pages, 10 figures

In the spinel compound GeCo$_2$O$_4$, the Co$^{2+}$ pyrochlore sublattice presents remarkable magnetic field-induced behaviors that we unveil through neutron and X-ray single-crystal diffraction. The N\'eel ordered magnetic phase is entered through a structural lowering of the cubic symmetry. In this phase, when a magnetic field is applied along a 2-fold cubic direction, a spin-flop transition of one fourth of the magnetic moments releases the magnetic frustration and triggers magnetostructural effects. At high field, these ultimately lead to an unusual spin reorientation associated to structural changes.

We present an experimental study of the quantum spin ice candidate pyrochlore coumpound \przr\ by means of magnetization measurements, specific heat and neutron scattering up to 12 T and down to 60 mK. When the field is applied along the $[111]$ and $[1\bar{1}0]$ directions, ${\bf k}=0$ field induced structures settle in. We find that the ordered moment rises slowly, even at very low temperature, in agreement with macroscopic magnetization. Interestingly, for $H \parallel [1\bar{1}0]$, the ordered moment appears on the so called $\alpha$ chains only. The spin excitation spectrum is essentially {\it inelastic} and consists in a broad flat mode centered at about 0.4 meV with a magnetic structure factor which resembles the spin ice pattern. For $H \parallel [1\bar{1}0]$ (at least up to 2.5 T), we find that a well defined mode forms from this broad response, whose energy increases with $H$, in the same way as the temperature of the specific heat anomaly. We finally discuss these results in the light of mean field calculations and propose a new interpretation where quadrupolar interactions play a major role, overcoming the magnetic exchange. In this picture, the spin ice pattern appears shifted up to finite energy because of those new interactions. We then propose a range of acceptable parameters for \przr\, that allow to reproduce several experimental features observed under field. With these parameters, the actual ground state of this material would be an antiferroquadrupolar liquid with spin-ice like excitations.

Fractionalised excitations that emerge from a many body system have revealed rich physics and concepts, from composite fermions in two-dimensional electron systems, revealed through the fractional quantum Hall effect, to spinons in antiferromagnetic chains and, more recently, fractionalisation of Dirac electrons in graphene and magnetic monopoles in spin ice. Even more surprising is the fragmentation of the degrees of freedom themselves, leading to coexisting and a priori independent ground states. This puzzling phenomenon was recently put forward in the context of spin ice, in which the magnetic moment field can fragment, resulting in a dual ground state consisting of a fluctuating spin liquid, a so-called Coulomb phase, on top of a magnetic monopole crystal. Here we show, by means of neutron scattering measurements, that such fragmentation occurs in the spin ice candidate Nd$_2$Zr$_2$O$_7$. We observe the spectacular coexistence of an antiferromagnetic order induced by the monopole crystallisation and a fluctuating state with ferromagnetic correlations. Experimentally, this fragmentation manifests itself via the superposition of magnetic Bragg peaks, characteristic of the ordered phase, and a pinch point pattern, characteristic of the Coulomb phase. These results highlight the relevance of the fragmentation concept to describe the physics of systems that are simultaneously ordered and fluctuating., Comment: accepted in Nature Physics

We present an experimental study of the pyrochlore coumpound Nd2Zr2O7 by means of neutron scattering and magnetization measurements down to 90 mK. The Nd$^{3+}$ magnetic moments exhibit a strong local $\langle$111$\rangle$ Ising anisotropy together with a dipolar-octupolar nature, different from the standard Kramers-doublet studied so far. We show that, despite the positive Curie-Weiss temperature, \ndzr\ undergoes a transition around 285 mK towards an all-in$-$all-out antiferromagnetic state. We establish the $(H,T)$ phase diagram in the three directions of the applied field and reveal a metamagnetic transition around 0.1 T. The strongly reduced ordered magnetic moment as well as the unexpected shape of the magnetization curves demonstrate that Nd2Zr2O7 , is not a standard Ising antiferromagnet. We propose that the peculiar nature of the Nd doublet combined with competing interactions explain these findings.

We report neutron diffraction experiments performed in the tetragonal antiferromagnetic heavy fermion system CeRhIn$_{5-x}$Sn$_{x}$ in its ($x$, $T$) phase diagram up to the vicinity of the critical concentration $x_c$ $\approx$ 0.40, where long range magnetic order is suppressed. The propagation vector of the magnetic structure is found to be $\bf{k_{IC}}$=(1/2, 1/2, $k_l$) with $k_l$ increasing from $k_l$=0.298 to $k_l$=0.410 when $x$ increases from $x$=0 to $x$=0.26. Surprisingly, for $x$=0.30, the order has changed drastically and a commensurate antiferromagnetism with $\bf{k_{C}}$=(1/2, 1/2, 0) is found. This concentration is located in the proximity of the quantum critical point where superconductivity is expected., Comment: 5 pages, 5 figures, submitted to Phys. Rev. B

Field-induced magnetic ordering in the structurally disordered quantum magnets Ni(Cl$_{1-x}$Br$_x$)$_2$$\cdot$4SC(NH$_2$)$_2$, $x=8$% and 13%, is studied by means of neutron diffraction. The order parameter critical exponent is found to be very close to its value $\beta=0.5$ expected for magnetic Bose-Einstein condensation in the absence of disorder. This result applies to temperatures down to 40 mK, and a 1 T range in magnetic field. The crossover exponent is found to be $\phi \sim 0.4$, for temperature ranges as small as 300 mK. Possible reasons for a discrepancy with recent numerical simulations and bulk measurements are discussed., Comment: submitted to PRB

We have studied the field-induced magnetic structures of Tb2Ti2O7 pyrochlore by single-crystal neutron diffraction under a field applied along the [111] local anisotropy axis, up to H=12T and down to T=40mK. We collected a hundred magnetic Bragg peaks for each field and temperature value and refined the magnetic structures with k=0 propagation vector by performing a symmetry analysis in the space group R-3m, reducing the number of free parameters to three only. We observe a gradual reorientation of the Tb magnetic moments towards the field direction, close to a "3-in, 1-out / 1-in, 3-out" spin structure in the whole field range 0.05-12T. We perform a quantitative comparison with mean-field calculations and we propose the presence of a low-temperature dynamic symmetry breaking of the local trigonal symmetry, akin to a dynamic Jahn-Teller effect, i.e. preserving the overall cubic symmetry. We discuss the possible origin of this off-diagonal mixing term in the crystal field hamiltonian in terms of quadrupole-quadrupole interaction or magneto-elastic effects., Comment: 10 pages, 11 figures, 1 table, submitted for publication

We present macroscopic and neutron diffraction data on multiferroic lightly Co-doped Ni$_3$V$_2$O$_8$. Doping Co into the parent compound suppresses the sequence of four magnetic phase transitions and only two magnetically ordered phases, the paraelectric high temperature incommensurate (HTI) and ferroelectric low temperature incommensurate (LTI), can be observed. Interestingly, the LTI multiferroic phase with a spiral (cycloidal) magnetic structure is stabilized down to at least 1.8 K, which could be revealed by measurements of the electric polarization and confirmed by neutron diffraction on single crystal samples. The extracted magnetic moments of the LTI phase contain besides the main exchange also fine components of the cycloid allowed by symmetry which result in a small amplitude variation of the magnetic moments along the cycloid propagation due to the site-dependent symmetry properties of the mixed representations. In the HTI phase a finite imaginary part of the spine magnetic moment could be deduced yielding a spin cycloid instead of a purely sinusoidal structure with an opposite spin chirality for different spine spin chains. The magnetic ordering of the cross-tie sites in both phases is different in comparison to the respective ones in the pure Ni compound. A wider temperature stability range of the HTI phase has been observed in comparison to Ni$_3$V$_2$O$_8$ which can be explained by an additional single-ion easy-axis anisotropy due to Co-doping. The larger incommensurability of the Co-doped compounds yields a larger ratio between the competing next-nearest neighbour and nearest neighbour interaction, which is $J_2/J_1$=0.43 (0.47) for a doping level of 7% (10%) Co compared to 0.39 in the parent compound., Comment: 9 pages, 6 figures

We present a detailed low-temperature investigation of the statics and dynamics of the anions and methyl groups in the organic conductors (TMTSF)$_2$PF$_6$ and (TMTSF)$_2$AsF$_6$ (TMTSF : tetramethyl-tetraselenafulvalene). The 4 K neutron scattering structure refinement of the fully deuterated (TMTSF)$_2$PF$_6$-D12 salt allows locating precisely the methyl groups at 4 K. This structure is compared to the one of the fully hydrogenated (TMTSF)$_2$PF$_6$-H12 salt previously determined at the same temperature. Surprisingly it is found that deuteration corresponds to the application of a negative pressure of 5 x 10$^2$ MPa to the H12 salt. Accurate measurements of the Bragg intensity show anomalous thermal variations at low temperature both in the deuterated PF$_6$ and AsF$_6$ salts. Two different thermal behaviors have been distinguished. Low-Bragg-angle measurements reflect the presence of low-frequency modes at characteristic energies {\theta}$_E$ = 8.3 K and {\theta}$_E$ = 6.7 K for the PF$_6$-D12 and AsF$_6$-D12 salts, respectively. These modes correspond to the low-temperature methyl group motion. Large-Bragg-angle measurements evidence an unexpected structural change around 55 K which probably corresponds to the linkage of the anions to the methyl groups via the formation of F...D-CD2 bonds observed in the 4 K structural refinement. Finally we show that the thermal expansion coefficient of (TMTSF)$_2$PF$_6$ is dominated by the librational motion of the PF$_6$ units. We quantitatively analyze the low-temperature variation of the lattice expansion via the contribution of Einstein oscillators, which allows us to determine for the first time the characteristic frequency of the PF6 librations: {\theta}$_E$ = 50 K and {\theta}$_E$ = 76 K for the PF$_6$-D12 and PF$_6$-H12 salts, respectively.

Er2Ti2O7 is believed to be a realization of an XY antiferromagnet on a frustrated lattice of corner-sharing regular tetrahedra. It is presented as an example of the order-by-disorder mechanism in which fluctuations lift the degeneracy of the ground state, leading to an ordered state. Here we report detailed measurements of the low temperature magnetic properties of Er2Ti2O7, which displays a second-order phase transition at T_N \simeq 1.2 K with coexisting short- and long-range orders. Magnetic-susceptibility studies show that there is no spin-glass-like irreversible effect. Heat-capacity measurements reveal that the paramagnetic critical exponent is typical of a 3-dimensional XY magnet while the low-temperature specific heat sets an upper limit on the possible spin-gap value and provides an estimate for the spin-wave velocity. Muon spin relaxation measurements show the presence of spin dynamics in the nanosecond time scale down to 21 mK. This time range is intermediate between the shorter time characterizing the spin dynamics in Tb2Sn2O7, which also displays long- and short-range magnetic order, and the time scale typical of conventional magnets. Hence the ground state is characterized by exotic spin dynamics. We determine the parameters of a symmetry-dictated Hamiltonian restricted to the spins in a tetrahedron, by fitting the paramagnetic diffuse neutron scattering intensity for two reciprocal lattice planes. These data are recorded in a temperature region where the assumption that the correlations are limited to nearest neighbors is fair., Comment: 16 pages, 16 figures

Neutron diffraction and calorimetric measurements are used to study the field-induced quantum phase transition in piperazinium-Cu$_2$(Cl$_{1-x}$Br$_x$)$_6$ ($x=0$, x=3.5% and x=7.5%), a prototypical quantum antiferromagnet with random bonds. The critical indexes $\phi$ and $\beta$ are determined. The findings contradict some original predictions for Bose Glass based on the assumption $z=d$, but are consistent with recent theoretical results implying $z

We show that a crystal of mesoscopic Fe8 single molecule magnets is an experimental realization of the Quantum Ising Phase Transition (QIPT) model in a transverse field, with dipolar interactions. Quantum annealing has enabled us to explore the QIPT at thermodynamical equilibrium. The phase diagram and critical exponents we obtain are compared to expectations for the mean-field QIPT Universality class., Comment: 5 pages 4 figures

We report a polarized neutron diffraction study conducted to reveal the nature of the weak ferromagnetic moment in the superconducting ferromagnet UCoGe. We find that the ordered moment in the normal phase in low magnetic fields (B // c) is predominantly located at the U atom and has a magnitude of about 0.1 muB at 3 T, in agreement with bulk magnetization data. By increasing the magnetic field the U moment grows to about 0.3 muB in 12 T and most remarkably, induces a substantial moment (about 0.2 muB) on the Co atom directed antiparallel to the U moment. The anomalous polarizability of the Co 3d orbitals is unique among uranium intermetallics and might reflect the proximity to a magnetic quantum critical point of UCoGe in zero field., Comment: 3 figures, accepted for Phys. Rev. B, Rapid Communication

We present a combination of ab initio calculations, magnetic Compton scattering and polarized neutron experiments, which elucidate the density distribution of unpaired electrons in the kagome staircase system Co3V2O8. Ab initio wave functions were used to calculate the spin densities in real and momentum space, which show good agreement with the respective experiments. It has been found that the spin polarized orbitals are equally distributed between the t2g and the eg levels for the spine (s) Co ions, while the eg orbitals of the cross-tie (c) Co ions only represent 30% of the atomic spin density. Furthermore, the results reveal that the magnetic moments of the cross-tie Co ions, which are significantly smaller than those of the spine Co ions in the zero-field ferromagnetic structure, do not saturate by applying an external magnetic field of 2 T along the easy axis a, but that the increasing bulk magnetization originates from induced magnetic moments on the O and V sites. The refined individual magnetic moments are mu(Co_c)=1.54(4) mu_B, mu(Co_s)=2.87(3) mu_B, mu(V)=0.41(4) mu_B, mu(O1)=0.05(5) mu_B, mu(O2)=0.35(5) mu_B, and; mu(O3)=0.36(5) mu_B combining to the same macroscopic magnetization value, which was previously only attributed to the Co ions.

The entire magnetic phase diagram of the quasi two dimensional (2D) magnet on a distorted triangular lattice KFe(MoO4)2 is outlined by means of magnetization, specific heat, and neutron diffraction measurements. It is found that the spin network breaks down into two almost independent magnetic subsystems. One subsystem is a collinear antiferromagnet that shows a simple spin-flop behavior in applied fields. The other is a helimagnet that instead goes through a series of exotic commensurate-incommensurate phase transformations. In the various phases one observes either true 3D order or quasi-2D order. The experimental findings are compared to theoretical predictions found in literature, Comment: 4 pages, 4 figures

Neutron scattering is used to study magnetic field induced ordering in the quasi-1D quantum spin-tube compound Sul--Cu$_2$Cl$_4$ that in zero field has a non-magnetic spin-liquid ground state. The experiments reveal an incommensurate chiral high-field phase stabilized by a geometric frustration of the magnetic interactions. The measured critical exponents $\beta\approx0.235$ and $\nu\approx0.34$ at $H_c\approx3.7$ T point to an unusual sub-critical scaling regime and may reflect the chiral nature of the quantum critical point., Comment: 4 pages

Inelastic and elastic neutron scattering is used to study spin correlations in the quasi-one dimensional quantum antiferromagnet IPA-CuCl3 in strong applied magnetic fields. A condensation of magnons and commensurate transverse long-range ordering is observe at a critical filed $H_c=9.5$ T. The field dependencies of the energies and polarizations of all magnon branches are investigated both below and above the transition point. Their dispersion is measured across the entire 1D Brillouin zone in magnetic fields up to 14 T. The critical wave vector of magnon spectrum truncation [Masuda et al., Phys. Rev. Lett. 96, 047210 (2006)] is found to shift from h_c 0.35 at H>H_c. A drastic reduction of magnon bandwidths in the ordered phase [Garlea et al., Phys. Rev. Lett. 98, 167202 (2007)] is observed and studied in detail. New features of the spectrum, presumably related to this bandwidth collapse, are observed just above the transition field.