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The discovery of chiral helical magnetism (CHM) in Cr$_{1/3}$NbS$_2$ and the stabilization of a chiral soliton lattice (CSL) has attracted considerable interest in view of their potential technological applications. However, there is an ongoing debate regarding whether the sister compound, Mn$_{1/3}$NbS$_2$, which shares the same crystal structure, exhibits similar nontrivial properties which rely on the stabilization of the lack of inversion symmetry at the magnetic ion. In this study, we conduct a comprehensive investigation of the magnetically ordered states of both compounds, using $^{53}$Cr, $^{55}$Mn and $^{93}$Nb nuclear magnetic resonance. Our results, supported by density functional calculations, detect in a high-quality single crystal of Cr$_{1/3}$NbS$_2$ all the signatures of the monoaxial CHM in a magnetic field, identifying it as a textbook NMR case. The detailed understanding of this prototypic behavior provides a reference for Mn$_{1/3}$NbS$_2$. Despite the much larger density of specific defects in this second single crystal, we confirm the presence of a CHM phase in the Mn compound, characterized by a very large critical field for the forced ferromagnetic phase ($\approx 5$ T for H$\parallel\hat c$)., Comment: 10 pages, 7 figures, Supplemental MAterial

We present local and nonlocal electrical transport measurements of the correlated insulator FeSb$_2$. By employing wiring configurations that delineate between bulk- and surface-dominated conduction, we reveal the formation of a metallic surface state in FeSb$_2$ for temperatures $\lessapprox 5$~K. This result is corroborated by an angular rotation study of this material's magnetotransport, which also shows signatures of the transition from bulk- to surface-dominated conduction over the same temperature interval as the local/nonlocal transport divergence. Notable similarities with the topological Kondo insulator candidate SmB$_6$ are discussed.

BiTeI is a polar semiconductor with strong spin-orbit coupling (SOC) that produces large Rashba spin splitting. Due to its potential utility in spintronics and magnetoelectrics, it is essential to understand how defects impact the spin transport in this material. Using scanning tunneling microscopy and spectroscopy, we image ring-like charging states of single-atom defects on the iodine surface of BiTeI. We observe nanoscale variations in the Rashba energy around each defect, which we correlate with the local electric field extracted from the bias dependence of each ring radius. Our data demonstrate the local impact of atomic defects on the Rashba effect, which is both a challenge and an opportunity for the development of future nanoscale spintronic devices.

Magnetometry and magnetoresistance (MR) data taken on the van der Waals ferromagnet Fe$_{3-x}$GeTe$_2$ (FGT) reveal three distinct contributions to the MR: a linear negative component, a contribution from closed Fermi-surface orbits, and a $H^2$ enhancement linked to a non-coplanar spin arrangement. Contrary to earlier studies on FGT, by accounting for the field dependence of the anomalous Hall effect, we find that the ordinary Hall coefficient decreases markedly below 80 K, indicating a significant change in character of the electrons and holes on the Fermi surface at this temperature. The resulting altered ground state eventually causes the Hall coefficient to reverse sign at 35 K. Our Hall data support the proposal that Kondo-lattice behavior develops in this $d$-electron material below 80 K. Additional evidence comes from the negative linear component of the MR, which arises from electron-magnon scattering with an atypical temperature dependence attributable to the onset of Kondo screening.

We report high-resolution dilatometry studies on single crystals of the Shastry-Sutherland-lattice magnet NdB$_4$ supported by specific heat and magnetometry data. Our dilatometric studies evidence pronounced anomalies at the phase boundaries which imply strong magneto-elastic coupling. The evolution of the three zero-field phase transitions separating distinct antiferromagnetic phases at $TN=17.2$~K, $TIT=6.8$~K and $TLT=4.8$~K can thus be traced in applied magnetic fields which provides the magnetic phase diagrams for $B\parallel c$ up to 15~T and for $B\parallel [110]$ up to 35~T. New in-field phases are discovered for both field directions and already known phases are confirmed. In particular, phase boundaries between different phases are unambiguously shown by sign changes of observed anomalies and corresponding changes in uniaxial pressure effects. For $B||c$, we find a 1/4-magnetization plateau in addition to a previously reported plateau at 1/5 of the saturation magnetization. TN increases for $B\parallel c$ in fields up to 15~T implying that magnetic moments of the all-in/all-out structure in the high temperature AFM ordered phase are driven towards the $c$ axis in high magnetic fields. Uniaxial pressure dependencies ${\partial}T_{\mathrm{crit}}/{\partial}p_{\mathrm{c}}$ of the phase transition temperatures for magnetic fields and pressure applied along the $c$ axis are derived from the data.

The recent discovery of the persistence of long-range magnetic order when van der Waals layered magnets are thinned towards the monolayer limit has provided a tunable platform for the engineering of novel magnetic structures and devices. Here, we study the evolution of the electronic structure of CrGeTe$_3$ as a function of electron doping in the surface layer. From angle-resolved photoemission spectroscopy, we observe spectroscopic fingerprints that this electron doping drives a marked increase in $T_\mathrm{C}$, reaching values more than double that of the undoped material, in agreement with recent studies using electrostatic gating. Together with density functional theory calculations and Monte Carlo simulations, we show that, surprisingly, the increased $T_\mathrm{C}$ is mediated by the population of spin-minority Cr $t_{2g}$ states, forming a half-metallic 2D electron gas at the surface. We show how this promotes a novel variant of double exchange, and unlocks a significant influence of the Ge -- which was previously thought to be electronically inert in this system -- in mediating Cr-Cr exchange., Comment: 10 pages including supplementary information

Mn$_3$Si$_2$Te$_6$ is a rare example of a layered ferrimagnet. It has recently been shown to host a colossal angular magnetoresistance as the spin orientation is rotated from the in- to out-of-plane direction, proposed to be underpinned by a topological nodal-line degeneracy in its electronic structure. Nonetheless, the origins of its ferrimagnetic structure remain controversial, while its experimental electronic structure, and the role of correlations in shaping this, are little explored to date. Here, we combine x-ray and photoemission-based spectroscopies with first-principles calculations, to probe the elemental-selective electronic structure and magnetic order in Mn$_3$Si$_2$Te$_6$. Through these, we identify a marked Mn-Te hybridisation, which weakens the electronic correlations and enhances the magnetic anisotropy. We demonstrate how this strengthens the magnetic frustration in Mn$_3$Si$_2$Te$_6$, which is key to stabilising its ferrimagnetic order, and find a crucial role of both exchange interactions extending beyond nearest-neighbours and anti-symmetric exchange in dictating its ordering temperature. Together, our results demonstrate a powerful methodology of using experimental electronic structure probes to constrain the parameter space for first-principles calculations of magnetic materials, and through this approach, reveal a pivotal role played by covalency in stabilising the ferrimagnetic order in Mn$_3$Si$_2$Te$_6$.

The competition between magnetic order and Kondo effect is essential for the rich physics of heavy fermion systems. Nevertheless, how such competition is manifested in the quasiparticle bands in a real periodic lattice remains elusive in spectroscopic experiments. Here we report a high-resolution photoemission study of the antiferromagnetic Kondo lattice system CeCoGe3 with a high TN1 of 21K. Our measurements reveal a weakly dispersive 4f band at the Fermi level near the Z point, arisingfrom moderate Kondo effect. The intensity of this heavy 4f band exhibits a logarithmic increase with lowering temperature and begins to deviate from this Kondo-like behavior below 25 K, just above TN1, and eventually ceases to grow below 12 K. Our work provides direct spectroscopic evidence for the competition between magnetic order and the Kondo effect in a Kondo lattice system with local-moment antiferromagnetism, indicating a distinct scenario for the microscopic coexistence and competition of these phenomena, which might be related to the real-space modulation., Comment: 7 pages, 4 figures

Layered transition-metal dichalcogenides are proposed as building blocks for van der Waals (vdW) heterostructures due to their graphene-like two dimensional structure. For this purpose, a magnetic semiconductor could represent an invaluable component for various spintronics and topotronics devices. Here, we combine different local magnetic probe spectroscopies with angle-resolved photoemission and density-functional theory calculations to show that 2H-MoTe2 is on the verge of becoming magnetic. Our results present clear evidence that the magnetism can be "switched on" by a hydrogen-like impurity. We also show that this magnetic state survives up to the free surface region, demonstrating the material's potential applicability as a magnetic component for thin-film heterostructures., Comment: 17 pages, 13 figures, including supplementary

Magnetic skyrmions are vortex-like, swirls of magnetisation whose topological protection and particle-like nature have suggested them to be suitable for a number of novel spintronic devices. One such application is skyrmionic computing, which has the advantage over conventional schemes due to the amalgamation of logic calculations and data storage. Using small-angle neutron scattering from Cu2OSeO3, and applying electric and magnetic fields, we find that the direction of the skyrmion-coexisting conical states can be manipulated by varying the electric field, and explain this using a free energy approach. Our findings unlock the prospect of creating a number of skyrmion devices which may constitute part of a skyrmion computer, as the direction of a skyrmion within a nanosized racetrack can be manipulated into different channels by controllably changing the direction of the localised conical state. We provide time-dependant micromagnetic simulations to demonstrate such a device: a skyrmion double transistor.

The quest to understand the nature of the electronic state in SmB6 has been challenging, perplexing and surprising researchers for over half a century. In the theoretically predicted topological Kondo insulator SmB6, the nature of the bulk electronic structure is not characterised unambiguously by quantum oscillations due to contrary interpretations. One simple definition of an electrical insulator is a material that lacks a Fermi surface and here we report the results of our investigation into its existence in SmB6 by Compton scattering. Compton scattering measures occupied electron momentum states, is bulk sensitive due to the high energy of the incoming photons and is also an ultra-fast probe of the correlated many-body electron wavefunction. Remarkably, direct evidence for a three-dimensional remnant Fermi surface is observed. However, a further dichotomy is raised in that the full occupancy expected of a conventional metal is not reproduced. Our observation of a remnant Fermi surface using a momentum-resolved probe provides significant new evidence that the paradigm of a bulk insulator is not robust for SmB6., Comment: 14 pages, 10 figures (Supplementary information included)

We report results from an in--plane and out--of--plane impedance study on SmB$_6$ single crystals, performed at low temperatures and over a wide frequency range. A universal equivalent circuit describes the dielectric behavior of this system across the transition, from surface to bulk dominated electrical conduction between 2 and 10 K. We identify the resistive, capacitive, and inductive contributions to the impedance. The equivalent inductance, obtained from fits to experimental data, drops drastically as the bulk starts to control electrical conduction upon increasing temperature. SmB$_6$ single crystals also show current--controlled negative differential resistance at low temperatures, which is brought about by Joule heating. This feature, in addition to inductive and capacitive contributions to the impedance, can give rise to the self--sustained voltage oscillations observed below 5 K (Stern {\it et al.}, Phys. Rev. Lett. {\bf 116}, 166603 (2016))., Comment: 14 pages, 6 figures

Since its discovery as a Kondo insulator 50 years ago, SmB6 recently received a revival of interest due to detection of unexpected quantum oscillations in the insulating state, discovery of disorder-immune bulk transport, and proposals of correlation-driven topological physics. While recent transport results attribute the anomalous low temperature conduction to two-dimensional surface states, important alternatives, such as conduction channel residing in one-dimensional dislocation lines, have not been adequately explored. Here we study SmB6 with scanning microwave impedance microscopy and uncover evidence for conducting one-dimensional states terminating at surface step edges. These states remain conducting up to room temperature, indicating unusual robustness against scattering and an unconventional origin. Our results bring to light a heretofore undetected conduction route in SmB6 that contributes to the low temperature transport. The unique scenario of intrinsic one-dimensional conducting channels in a highly insulating correlated bulk offers a one-dimensional platform that may host exotic physics., Comment: Upon further follow-up studies, we discovered additional data in different parameter spaces that weakened our arguments. While this does not preclude the existence of 1-D conducting states, we feel that our previous supporting arguments are rendered ineffective, and we must suspend and withdraw our manuscript at this point

Modern Superconducting QUantum Interference Devices (SQUIDs) are commonly fabricated from either Al or Nb electrodes, with an in-situ oxidation process to create a weak link between them. However, common problems of such planar nano- and micro-SQUIDs are hysteretic current-voltage curves, and a shallow flux modulation depth. Here, we demonstrate the formation of both Josephson junctions and SQUIDs using a dry transfer technique to stack and deterministically misalign flakes of NbSe$_{2}$; allowing one to overcome these issues. The Josephson dynamics of the resulting twisted NbSe$_{2}$-NbSe$_{2}$ junctions are found to be sensitive to the misalignment angle of the crystallographic axes. A single lithographic process was then implemented to shape the Josephson junction into a SQUID geometry with typical loop areas of $\simeq$ 25 $\mu m^{2}$ and weak links $\simeq$ 600 nm wide. These devices display large stable current and voltage modulation depths of up to $\Delta I_{c} \simeq$ 75$\%$ and $\Delta V \simeq$ 1.4 mV respectively., Comment: 12 pages, 6 figures

We report high-resolution capacitance dilatometry studies on the uniaxial length changes in a NdB$_4$ single crystal. The evolution of magnetically ordered phases below $T_{\rm N}$= 17.2~K (commensurate antiferromagnetic phase, cAFM), $T_{\rm IT}$= 6.8~K (intermediate incommensurate phase, IT), and $T_{\rm LT}$= 4.8~K (low-temperature phase, LT) is associated with pronounced anomalies in the thermal expansion coefficients. The data imply significant magneto-elastic coupling and evidence of a structural phase transition at $T_{\rm LT}$ . While both cAFM and LT favor structural anisotropy $\delta$ between in-plane and out-of-plane length changes, it competes with the IT-type of order, i.e., $\delta$ is suppressed in that phase. Notably, finite anisotropy well above $T_{\rm N}$ indicates short-range correlations which are, however, of neither cAFM, IT, nor LT-type. Gr\"uneisen analysis of the ratio of thermal expansion coefficient and specific heat enables the derivation of uniaxial as well as hydrostatic pressure dependencies. While $\alpha$/$c_{\rm p}$ evidences a single dominant energy scale in LT, our data imply precursory fluctuations of a competing phase in IT and cAFM, respectively. Our results suggest the presence of orbital degrees of freedom competing with cAFM and successive evolution of a magnetically and orbitally ordered ground state.

We investigate the roles of disorder on low-temperature transport in SmB$_6$ crystals grown by both the Al flux and floating zone methods. We used the inverted resistance method with Corbino geometry to investigate whether low-temperature variations in the standard resistance plateau arises from a surface or a bulk channel in floating zone samples. The results show significant sample-dependent residual bulk conduction, in contrast to smaller amounts of residual bulk conduction previously observed in Al flux grown samples with Sm vacancies. We consider hopping in an activated impurity band as a possible source for the observed bulk conduction, but it is unlikely that the large residual bulk conduction seen in floating zone samples is solely due to Sm vacancies. We therefore propose that one-dimensional defects, or dislocations, contribute as well. Using chemical etching, we find evidence for dislocations in both flux and floating zone samples, with higher dislocation density in floating zone samples than in Al flux grown samples. In addition to the possibility of transport through one-dimensional dislocations, we also discuss our results in the context of recent theoretical models of SmB$_6$., Comment: 22 pages, 4 figures

We present an aberration corrected scanning transmission electron microscopy (ac-STEM) analysis of the perovskite (LaFeO3) and pyrochlore (Yb2Ti2O7 and Pr2Zr2O7) oxides and demonstrate that both the shape and contrast of visible atomic columns in annular dark-field (ADF) images are sensitive to the presence of nearby atoms of low atomic number (e.g. oxygen). We show that point defects (e.g. oxygen vacancies), which are invisible - or difficult to observe due to limited sensitivity - in X-ray and neutron diffraction measurements, are the origin of the complex magnetic ground state of pyrochlore oxides. In addition, we present, for the first time, a method by which light atoms can be resolved in quantitative ADF-STEM images. Using this method, we resolved oxygen atoms in perovskite and pyrochlore oxides., Comment: 18 pages and 7 figures plus supplementary information

The wealth of structural phases seen in the rare-earth disilicate compounds promises an equally rich range of interesting magnetic properties. We report on the crystal growth by the optical floating zone method of members of the rare-earth disilicate family, $R_{2}$Si$_{2}$O$_{7}$ (with $R=$ Er, Ho, and Tm). Through a systematic study, we have optimised the growth conditions for Er$_{2}$Si$_{2}$O$_{7}$. We have grown, for the first time using the floating zone method, crystal boules of Ho$_{2}$Si$_{2}$O$_{7}$ and Tm$_{2}$Si$_{2}$O$_{7}$ compounds. We show that the difficulties encountered in the synthesis of polycrystalline and single crystal samples are due to the similar thermal stability ranges of different rare-earth silicate compounds in the temperature-composition phase diagrams of the $R$-Si-O systems. The addition of a small amount of SiO$_{2}$ excess allowed the amount of impurity phases present in the powder samples to be minimised. The phase composition analysis of the powder X-ray diffraction data collected on the as-grown boules revealed that they were of single phase, except in the case of thulium disilicate, which comprised of two phases. All growths resulted in multi-grain boules, from which sizable single crystals could be isolated. The optimum conditions used for the synthesis and crystal growth of polycrystalline and single crystal $R_{2}$Si$_{2}$O$_{7}$ materials are reported. Specific heat measurements of erbium and thulium disilicate compounds confirm an antiferromagnetic phase transition below $T_{\mathrm{N}}=$ 1.8 K for D-type Er$_{2}$Si$_{2}$O$_{7}$ and a Schottky anomaly centered around 3.5 K in C-type Tm$_{2}$Si$_{2}$O$_{7}$, suggesting the onset of short-range magnetic correlations. Magnetic susceptibility data of E-type Ho$_{2}$Si$_{2}$O$_{7}$ reveals an antiferromagnetic ordering of the Ho spins below $T_\mathrm{{N}}=$ 2.3 K., Comment: 35 pages, 13 figures, 4 tables

The finding of bulk quantum oscillations in the bulk Kondo insulator SmB$_6$, which has been proposed to be a correlated topological insulator, proved a considerable surprise. The subsequent measurement of bulk quantum oscillations in other correlated insulators including YbB$_{12}$ have lent support to our discovery of a class of unconventional insulators that are host to bulk quantum oscillations, of which SmB$_6$ was the first example. Here we perform a series of experiments to examine evidence for the intrinsic character of bulk quantum oscillations in floating zone-grown single crystals of SmB$_6$ that have been the subject of our quantum oscillation studies thus far. We present results of experiments including chemical composition analysis, magnetisation, thermal conductivity, electrical transport, and heat capacity on floating zone-grown single crystals of SmB$_6$, and a series of quantum oscillation experiments as a function of magnetic field, temperature, and magnetic field-orientation on single crystals of floating-zone grown SmB$_6$, LaB$_6$, and elemental Aluminium. Results of these experimental studies establish the intrinsic origin of quantum oscillations from the bulk of pristine floating zone-grown single crystals of SmB$_6$. The origin of the underlying bulk Fermi surface that bears close similarity with the unhybridised Fermi surface in metallic hexaborides despite the bulk insulating character of SmB$_6$ is thus at the heart of a theoretical mystery.

We report neutron scattering, magnetic susceptibility and Monte Carlo theoretical analysis to verify the short range nature of the magnetic structure and spin-spin correlations in a Yb$_3$Ga$_5$O$_{12}$ single crystal. The quantum spin state of Yb$^{3+}$ in Yb$_3$Ga$_5$O$_{12}$ is verified. The quantum spins organise into a short ranged emergent director state for T $<$ 0.4 K derived from anisotropy and near neighbour exchange. We derive the magnitude of the near neighbour exchange interactions $0.6\; {\rm K} < J_1 < 0.7\; {\rm K}, J_2 = 0.12$~K and the magnitude of the dipolar exchange interaction, $D$, in the range $0.18 < D < 0.21$ K. Certain aspects of the broad experimental dataset can be modelled using a $J_1D$ model with ferromagnetic near neighbour spin-spin correlations while other aspects of the data can be accurately reproduced using a $J_1J_2D$ model with antiferromagnetic near neighbour spin-spin correlation. As such, although we do not quantify all the relevant exchange interactions we nevertheless provide a strong basis for the understanding of the complex Hamiltonian required to fully describe the magnetic state of Yb$_3$Ga$_5$O$_{12}$., Comment: Main paper 10 pages, appendix 6 pages

The GaV$_4$S$_{8-y}$Se$_y$ $(y = 0$ to $8)$ family of materials have been synthesized in both polycrystalline and single crystal form, and their structural and magnetic properties thoroughly investigated. Each of these materials crystallizes in the $F\bar{4}3m$ space group at ambient temperature. However, in contrast to the end members GaV$_4$S$_8$ and GaV$_4$Se$_8$, that undergo a structural transition to the $R3m$ space group at 42 and 41 K respectively, the solid solutions $(y = 1$ to $7)$ retain cubic symmetry down to 1.5 K. In zero applied field the end members of the family order ferromagnetically at 13 K (GaV$_4$S$_8$) and 18 K (GaV$_4$Se$_8$), while the intermediate compounds exhibit a spin-glass-like ground state. We demonstrate that the magnetic structure of GaV$_4$S$_8$ shows localization of spins on the V cations, indicating that a charge ordering mechanism drives the structural phase transition. We conclude that the observation of both structural and ferromagnetic transitions in the end members of the series in zero field is a prerequisite for the stabilization of a skyrmion phase, and discuss how the absence of these transitions in the $y = 1$ to $7$ materials can be explained by their structural properties., Comment: Main text: 14 pages, 5 figures, 1 table. Supplementary information: 10 pages, 6 figures, 6 tables

We investigate the temperature-dependent electronic structure of the van der Waals ferromagnet, CrGeTe$_3$. Using angle-resolved photoemission spectroscopy, we identify atomic- and orbital-specific band shifts upon cooling through ${T_\mathrm{C}}$. From these, together with x-ray absorption spectroscopy and x-ray magnetic circular dichroism measurements, we identify the states created by a covalent bond between the Te ${5p}$ and the Cr ${e_g}$ orbitals as the primary driver of the ferromagnetic ordering in this system, while it is the Cr ${t_{2g}}$ states that carry the majority of the spin moment. The ${t_{2g}}$ states furthermore exhibit a marked bandwidth increase and a remarkable lifetime enhancement upon entering the ordered phase, pointing to a delicate interplay between localized and itinerant states in this family of layered ferromagnets.

After the theoretical prediction that SmB$_6$ is a topological Kondo insulator, there has been an explosion of studies on the SmB$_6$ surface. However, there is not yet an agreement on even the most basic quantities such as the surface carrier density and mobility. In this paper, we carefully revisit Corbino disk magnetotransport studies to find those surface transport parameters. We first show that subsurface cracks exist in the SmB$_6$ crystals, arising both from surface preparation and during the crystal growth. We provide evidence that these hidden subsurface cracks are additional conduction channels, and the large disagreement between earlier surface SmB$_6$ studies may originate from previous interpretations not taking this extra conduction path into account. We provide an update of a more reliable magnetotransport data than the previous one (Phys. Rev. B 92, 115110) and find that the orders-of-magnitude large disagreements in carrier density and mobility come from the surface preparation and the transport geometry rather than the intrinsic sample quality. From this magnetotransport study, we find an updated estimate of the carrier density and mobility of 2.71$\times$10$^{13}$ (1/cm$^2$) and 104.5 (cm$^{2}$/V$\cdot$sec), respectively. We compare our results with other studies of the SmB$_6$ surface. By this comparison, we provide insight into the disagreements and agreements of the previously reported angle-resolved photoemission spectroscopy, scanning tunneling microscopy, and magnetotorque quantum oscillations measurements.

Quantum spin ice is an appealing proposal of a quantum spin liquid - systems where the magnetic moments of the constituent electron spins evade classical long-range order to form an exotic state that is quantum entangled and coherent over macroscopic length scales. Such phases are at the edge of our current knowledge in condensed matter as they go beyond the established paradigm of symmetry-breaking order and associated excitations. Neutron scattering experiments on the pyrochlore material Pr$_2$Hf$_2$O$_7$ reveal signatures of a quantum spin ice state that were predicted by theory., Comment: Article in Swiss Neutron News, after R. Sibille et al. Nature Physics 14, 711- 715 (2018). https://sgn.web.psi.ch/sgn/snn.html

BaZrO3 is a perovskite that remains in the simple cubic phase at all temperatures, hence with no first-order Raman-active phonon mode allowed by symmetry. Yet, it exhibits an intense Raman spectrum with sharp and well-defined features. Here, we report the evolution of the Raman spectrum of BaZrO3 single crystals in a broad temperature range (4--1200~K) and discuss its origin with the support of detailed first-principle calculations of the lattice dynamics. Phonon calculations are performed not only for the cubic phase of BaZrO3, but also for the low-symmetry phases with octahedra tilts that have been suspected to exist at the nanoscale. We show that the Raman spectrum shows no direct evidence for these nanodomains, but can instead be explained by classical second-order Raman scattering. We provide an assignment of the dominant features to phonon modes combinations. In particular, we show that the high frequency range of the spectrum is dominated by overtones and shows an image of the phonon density of states corresponding to the stretching modes of the oxygen octahedra.

GdCo$_5$ may be considered as two sublattices - one of Gd and one of Co - whose magnetizations are in antiparallel alignment, forming a ferrimagnet. Substitution of nickel in the cobalt sublattice of GdCo$_5$ has been investigated to gain insight into how the magnetic properties of this prototype rare-earth/transition-metal magnet are affected by changes in the transition metal sublattice. Polycrystalline samples of GdCo$_{5-x}$Ni$_x$ for 0 $ \leq x \leq $ 5 were synthesized by arc melting. Structural characterization was carried out by powder x-ray diffraction and optical and scanning electron microscope imaging of metallographic slides, the latter revealing a low concentration of Gd$_2$(Co, Ni)$_7$ lamellae for $x \leq 2.5$. Compensation - i.e. the cancellation of the opposing Gd and transition metal moments is observed for $1 \leq x \leq 3$ at a temperature which increases with Ni content; for larger $x$, no compensation is observed below 360 K. A peak in the coercivity is seen at $x \approx 1$ at 10K coinciding with a minimum in the saturation magnetization. Density-functional theory calculations within the disordered local moment picture reproduce the dependence of the magnetization on Ni content and temperature. The calculations also show a peak in the magnetocrystalline anisotropy at similar Ni concentrations to the experimentally observed coercivity maximum., Comment: 12 pages, 12 figures, 2 tables

We present long-wavelength neutron diffraction data measured on both single crystal and polycrystalline samples of the skyrmion host material Cu$_{2}$OSeO$_{3}$. We observe magnetic satellites around the $(0\bar{1}1)$ diffraction peak not accessible to other techniques, and distinguish helical from conical spin textures in reciprocal space. We confirm successive transitions from helical to conical to field polarised ordered spin textures as the external magnetic field is increased. The formation of a skyrmion lattice with propagation vectors perpendicular to the field direction is observed in a region of the field-temperature phase diagram that is consistent with previous reports. Our measurements show that not only the field-polarised phase but also the helical ground state are made up of ferrimagnetic clusters instead of individual spins. These clusters are distorted Cu tetrahedra, where the spin on one Cu ion is anti-aligned with the spin on the three other Cu ions.

We present calculations and experimental measurements of the temperature-dependent magnetization of a single crystal of GdCo$_5$ in magnetic fields of order 60 T. At zero temperature the calculations, based on density-functional theory in the disordered-local-moment picture, predict a field-induced transition from an antiferromagnetic to a canted alignment of Gd and Co moments at 46.1 T. At higher temperatures the calculations find this critical field to increase along with the zero-field magnetization. The experimental measurements observe this transition to occur between 44-48 T at 1.4 K. Up to temperatures of at least 100 K, the experiments continue to observe the transition; however, at variance with the calculations, no strong temperature dependence of the critical field is apparent. We assign this difference to the inaccurate description of the zero-field magnetization of the calculations at low temperatures, due to the use of classical statistical mechanics. Correcting for this effect, we recover a consistent description of the high-field magnetization of GdCo$_5$ from theory and experiment., Comment: 11 pages, 4 figures. Data presented in this paper are available at http://wrap.warwick.ac.uk/103805

We present the results of a muon-spin spectroscopy investigation of GaV$_4$S$_{8-y}$Se$_{y}$ with $y=0, 2, 4$ and 8. Zero-field measurements suggest that GaV$_{4}$Se$_{8}$ and GaV$_{4}$S$_{8}$ have distinct magnetic ground states, with the latter material showing an anomalous temperature-dependence of the local magnetic field. It is not possible to evolve the magnetic state continuously between these two systems, with the intermediate $y=2$ and $4$ materials showing glassy magnetic behaviour at low temperature. The skyrmion lattice (SkL) phase is evident in the $y=0$ and 8 materials through an enhanced response of the muon-spin relaxation to the emergent dynamics that accompany the SkL. For our polycrystalline samples of GaV$_4$Se$_{8}$, this enhanced dynamic response is confined to a smaller region of the magnetic field-temperature phase diagram than the previous reports of the SkL in single crystals.

We report magnetic quantum oscillations measured using torque magnetisation in the Kondo insulator YbB$_{12}$ and discuss the potential origin of the underlying Fermi surface. Observed quantum oscillations as well as complementary quantities such as a finite linear specific heat capacity in YbB$_{12}$ exhibit similarities with the Kondo insulator SmB$_6$, yet also crucial differences. Small heavy Fermi sections are observed in YbB$_{12}$ with similarities to the neighbouring heavy fermion semimetallic Fermi surface, in contrast to large light Fermi surface sections in SmB$_6$ which are more similar to the conduction electron Fermi surface. A rich spectrum of theoretical models is suggested to explain the origin across different Kondo insulating families of a bulk Fermi surface potentially from novel itinerant quasiparticles that couple to magnetic fields, yet do not couple to weak DC electric fields., Comment: Journal of Physics: Condensed Matter (2018)

Magnetocrystalline anisotropy, the microscopic origin of permanent magnetism, is often explained in terms of ferromagnets. However, the best performing permanent magnets based on rare earths and transition metals (RE-TM) are in fact ferrimagnets, consisting of a number of magnetic sublattices. Here we show how a naive calculation of the magnetocrystalline anisotropy of the classic RE-TM ferrimagnet GdCo$_5$ gives numbers which are too large at 0 K and exhibit the wrong temperature dependence. We solve this problem by introducing a first-principles approach to calculate temperature-dependent magnetization vs. field (FPMVB) curves, mirroring the experiments actually used to determine the anisotropy. We pair our calculations with measurements on a recently-grown single crystal of GdCo$_5$, and find excellent agreement. The FPMVB approach demonstrates a new level of sophistication in the use of first-principles calculations to understand RE-TM magnets., Comment: 13 pages, 3 figures; Supplemental Information included in submission

We present a study of the magnetic-field effect on spin correlations in the charge ordered triangular Ising system LuFe2O4+{\delta} through single crystal neutron diffraction. In the absence of a magnetic field, the strong diffuse neutron scattering observed below the Neel temperature (TN = 240 K) indicates that LuFe2O4+{\delta} shows short-range, two-dimensional (2D) correlations in the FeO5 triangular layers, characterized by the development of a magnetic scattering rod along the 1/3 1/3 L direction, persisting down to 5 K. We also found that on top of the 2D correlations, a long range ferromagnetic component associated with the propagation vector k1 = 0 sets in at around 240 K. On the other hand, an external magnetic field applied along the c-axis effectively favours a three-dimensional (3D) spin correlation between the FeO5 bilayers evidenced by the increase of the intensity of satellite reflections with propagation vector k2 = (1/3, 1/3, 3/2). This magnetic modulation is identical to the charge ordered superstructure, highlighting the field-promoted coupling between the spin and charge degrees of freedom. Formation of the 3D spin correlations suppresses both the rod-type diffuse scattering and the k1 component. Simple symmetry-based arguments provide a natural explanation of the observed phenomenon and put forward a possible charge redistribution in the applied magnetic field., Comment: 9 pages, 6 figures

We present an investigation into the intrinsic magnetic properties of the compounds YCo5 and GdCo5, members of the RETM5 class of permanent magnets (RE = rare earth, TM = transition metal). Focusing on Y and Gd provides direct insight into both the TM magnetization and RE-TM interactions without the complication of strong crystal field effects. We synthesize single crystals of YCo5 and GdCo5 using the optical floating zone technique and measure the magnetization from liquid helium temperatures up to 800 K. These measurements are interpreted through calculations based on a Green's function formulation of density-functional theory, treating the thermal disorder of the local magnetic moments within the coherent potential approximation. The rise in the magnetization of GdCo5 with temperature is shown to arise from a faster disordering of the Gd magnetic moments compared to the antiferromagnetically aligned Co sublattice. We use the calculations to analyze the different Curie temperatures of the compounds and also compare the molecular (Weiss) fields at the RE site with previously published neutron scattering experiments. To gain further insight into the RE-TM interactions, we perform substitutional doping on the TM site, studying the compounds RECo4.5Ni0.5, RECo4Ni, and RECo4.5Fe0.5. Both our calculations and experiments on powdered samples find an increased/decreased magnetization with Fe/Ni doping, respectively. The calculations further reveal a pronounced dependence on the location of the dopant atoms of both the Curie temperatures and the Weiss field at the RE site., Comment: 13 figures, 1 table

In a quantum spin liquid, the magnetic moments of the constituent electron spins evade classical long-range order to form an exotic state that is quantum entangled and coherent over macroscopic length scales [1-2]. Such phases offer promising perspectives for device applications in quantum information technologies, and their study can reveal fundamentally novel physics in quantum matter. Quantum spin ice is an appealing proposal of one such state, in which the fundamental ground state properties and excitations are described by an emergent U(1) lattice gauge theory [3-7]. This quantum-coherent regime has quasiparticles that are predicted to behave like magnetic and electric monopoles, along with a gauge boson playing the role of an artificial photon. However, this emergent lattice quantum electrodynamics has proved elusive in experiments. Here we report neutron scattering measurements of the rare-earth pyrochlore magnet Pr$_2$Hf$_2$O$_7$ that provide evidence for a quantum spin ice ground state. We find a quasi-elastic structure factor with pinch points - a signature of a classical spin ice - that are partially suppressed, as expected in the quantum-coherent regime of the lattice field theory at finite temperature. Our result allows an estimate for the speed of light associated with magnetic photon excitations. We also reveal a continuum of inelastic spin excitations, which resemble predictions for the fractionalized, topological excitations of a quantum spin ice. Taken together, these two signatures suggest that the low-energy physics of Pr$_2$Hf$_2$O$_7$ can be described by emergent quantum electrodynamics. If confirmed, the observation of a quantum spin ice ground state would constitute a concrete example of a three-dimensional quantum spin liquid - a topical state of matter which has so far mostly been explored in lower dimensionalities., Comment: 15 pages, 3 figures

A study of the zero field and field induced magnetic states of the frustrated rare earth tetraboride, HoB$_4$, has been carried out using single crystal neutron diffraction complemented by magnetisation measurements. In zero field, HoB$_4$ shows magnetic phase transitions at $T_{\mathrm{N1}}$ = 7.1 K to an incommensurate state with a propagation vector ($\delta$, $\delta$, $\delta'$), where $\delta$ = 0.02 and $\delta'$ = 0.43 and at $T_{\mathrm{N2}}$ = 5.7 K to a non-collinear commensurate antiferromagnetic structure. Polarised neutron diffraction measurements in zero field have revealed that the incommensurate reflections, albeit much reduced in intensity, persist down to 1.5 K despite antiferromagnetic ordering at 5.7 K. At lower temperatures, application of a magnetic field along the $c$-axis initially re-establishes the incommensurate phase as the dominant magnetic state in a narrow field range, just prior to HoB$_4$ ordering with an up-up-down ferrimagnetic structure characterised by the $(h,k,\frac{1}{3})$-type reflections between 18 and 24 kOe. This field range is marked by the previously reported $M/M_{\mathrm{sat}}$= $\frac{1}{3}$ magnetisation plateau, which we also see in our magnetisation measurements. The region between 21 and 33 kOe is characterised by the increase in the intensity of the antiferromagnetic reflections, such as (100), the maximum of which coincides with the appearance of the narrow magnetisation plateau with $M/M_{\mathrm{sat}}\approx$ $\frac{3}{5}$. Further increase of the magnetic field results in the stabilisation of a polarised state above 33 kOe, while the incommensurate reflections are clearly present in all fields up to 59 kOe. We propose the $H-T$ phase diagram of HoB$_4$ for the $H \parallel c$ containing both stationary and transitionary magnetic phases which overlap and show significant history dependence., Comment: 9 pages, 10 figures, Accepted Physical Review B

Large single crystals of the pyrochlore Pr2Hf2O7 have been successfully grown by the floating zone technique using an optical furnace equipped with high power Xenon arc lamps. Structural investigations have been carried out by both synchrotron X-ray and neutron powder diffraction to establish the crystallographic structure of the materials produced. The magnetic properties of the single crystals have been determined for magnetic fields applied along different crystallographic axes. The results reveal that Pr2Hf2O7 is an interesting material for further investigations as a frustrated magnet. The high quality of the crystals produced make them ideal for detailed investigations, especially those using neutron scattering techniques., Comment: Accepted for publication in J. Phys.: Condens. Matter

The charge ordered structure of ions and vacancies characterizing rare-earth pyrochlore oxides serves as a model for the study of geometrically frustrated magnetism. The organization of magnetic ions into networks of corner-sharing tetrahedra gives rise to highly correlated magnetic phases with strong fluctuations, including spin liquids and spin ices. It is an open question how these ground states governed by local rules are affected by disorder. In the pyrochlore Tb$_2$Hf$_2$O$_7$, we demonstrate that the vicinity of the disordering transition towards a defective fluorite structure translates into a tunable density of anion Frenkel disorder while cations remain ordered. Quenched random crystal fields and disordered exchange interactions can therefore be introduced into otherwise perfect pyrochlore lattices of magnetic ions. We show that disorder can play a crucial role in preventing long-range magnetic order at low temperatures, and instead induces a strongly-fluctuating Coulomb spin liquid with defect-induced frozen magnetic degrees of freedom., Comment: 18 pages, 4 figures, + Supplementary Information (4 figures)

Accessing, controlling and understanding nanoscale friction and dissipation is a crucial issue in nanotechnology, where moving elements are central. Recently, ultra-sensitive noncontact pendulum Atomic Force Microscope (AFM) succeeded in detecting the electronic friction drop caused by the onset of superconductivity in Nb, raising hopes that a wider variety of mechanisms of mechanical dissipation arising from electron organization into different collective phenomena will become accessible through this unconventional surface probe. Among them, the driven phase dynamics of charge-density-waves (CDWs) represents an outstanding challenge as a source of dissipation. Here we report a striking multiplet of AFM dissipation peaks arising at nanometer distances above the surface of NbSe$_2$ - a layered compound exhibiting an incommensurate CDW. Each peak appears at a well defined tip-surface interaction force of the order of a nN, and persists until T=70K where CDW short-range order is known to disappear. A theoretical model is presented showing that the peaks are connected to tip-induced local 2$\pi$ CDW phase slips. Under the attractive potential of the approaching tip, the local CDW surface phase landscape deforms continuously until a series of 2$\pi$ jumps occur between different values of the local phase. As the tip oscillates to and fro, each slip gives rise to a hysteresis cycle, appearing at a selected distance, the dissipation corresponding to "pumping" in and out a local slip in the surface CDW phase of NbSe$_2$., Comment: 9 pages, 8 figures

We report the low temperature magnetic properties of the pyrochlore Pr$_2$Hf$_2$O$_7$. Polycrystalline and single-crystal samples are investigated using time-of-flight neutron spectroscopy and macroscopic measurements, respectively. The crystal-field splitting produces a non-Kramers doublet ground state for Pr$^{3+}$, with Ising-like anisotropy. Below 0.5 K ferromagnetic correlations develop, which suggests that the system enters a spin ice-like state associated with the metamagnetic behavior observed at $\mu_0H_c\sim2.4$~T. In this regime, the development of a discrete inelastic excitation in the neutron spectra indicates the appearance of spin dynamics which are likely related to cooperative quantum fluctuations., Comment: 7 pages, 5 figures, 1 table

In this paper, we present the observation of the electric field control on the charge-ordering and metamagnetic transitions during the magnetization measurements in a single crystal of Pr0.6Ca0.4MnO3 (PCMO). We have demonstrated that the complete melting of charge ordering can be realized in a single crystal of PCMO by applying a voltage as small as 2.5 V, which otherwise needs magnetic fields in excess of 11 T. The maximum change in magnetization with applied voltage occurs across the charge-ordering transition temperature (TCO = 235 K). Even though the electric field does not seem to affect the magnetic ordering, we see a clear evidence at low temperatures for the occurrence of the metamagnetic transitions at higher fields with the application of electric field.

We study the electronic structure of Bi(2)Se(3) employing high resolution photoemission spectroscopy and discover the dependence of the behavior of Dirac particles on surface terminations. The Dirac cone apex appears at different energies and exhibits contrasting shift on Bi and Se terminated surface with complex time dependence emerging from subtle adsorbed oxygen-surface atom interactions. These results uncover the surface states behavior of real systems possessing topologically ordered surface., Comment: 5 figures