Magnetic monopole density and antiferromagnetic domain control in spin-ice iridates.

Magnetically frustrated systems provide fertile ground for complex behaviour, including unconventional ground states with emergent symmetries, topological properties, and exotic excitations. A canonical example is the emergence of magnetic-charge-carrying quasiparticles in spin-ice compounds. Despite extensive work, a reliable experimental indicator of the density of these magnetic monopoles is yet to be found. Using measurements on single crystals of Ho2Ir2O7 combined with dipolar Monte Carlo simulations, we show that the isothermal magnetoresistance is highly sensitive to the monopole density. Moreover, we uncover an unexpected and strong coupling between the monopoles on the holmium sublattice and the antiferromagnetically ordered iridium ions. These results pave the way towards a quantitative experimental measure of monopole density and demonstrate the ability to control antiferromagnetic domain walls using a uniform external magnetic field, a key goal in the design of next-generation spintronic devices.

Chiral singlet superconductivity in the weakly correlated metal LaPt3P.

Chiral superconductors are novel topological materials with finite angular momentum Cooper pairs circulating around a unique chiral axis, thereby spontaneously breaking time-reversal symmetry. They are rather scarce and usually feature triplet pairing: a canonical example is the chiral p-wave state realized in the A-phase of superfluid He3. Chiral triplet superconductors are, however, topologically fragile with the corresponding gapless boundary modes only weakly protected against symmetry-preserving perturbations in contrast to their singlet counterparts. Using muon spin relaxation measurements, here we report that the weakly correlated pnictide compound LaPt3P has the two key features of a chiral superconductor: spontaneous magnetic fields inside the superconducting state indicating broken time-reversal symmetry and low temperature linear behaviour in the superfluid density indicating line nodes in the order parameter. Using symmetry analysis, first principles band structure calculation and mean-field theory, we unambiguously establish that the superconducting ground state of LaPt3P is a chiral d-wave singlet.

Investigation of the magnetic ground state of GaV4S8using powder neutron diffraction.

The magnetic ground state of polycrystalline Néel skyrmion hosting material GaV4S8has been investigated usingacsusceptibility and powder neutron diffraction. In the absence of an applied magnetic field GaV4S8undergoes a transition from a paramagnetic to a cycloidal state below 13 K and then to a ferromagnetic-like state below 6 K. With evidence fromacsusceptibility and powder neutron diffraction, we have identified the commensurate magnetic structure at 1.5 K, with ordered magnetic moments of 0.23(2) µBon the V1 sites and 0.22(1) µBon the V2 sites. These moments have ferromagnetic-like alignment but with a 39(8)° canting of the magnetic moments on the V2 sites away from the V4cluster. In the incommensurate magnetic phase that exists between 6 and 13 K, we provide a thorough and careful analysis of the cycloidal magnetic structure exhibited by this material using powder neutron diffraction.

Ir 5d-band derived superconductivity in LaIr3.

The superconducting properties of rhombohedral LaIr3 were examined using susceptibility, resistivity, heat capacity, and zero-field (ZF) and transverse-field (TF) muon spin relaxation and rotation ([Formula: see text]SR) measurements. The susceptibility and resistivity measurements confirm a superconducting transition below [Formula: see text] K. Two successive transitions are observed in the heat capacity data, one at [Formula: see text] K and a second at 1.2 K below [Formula: see text]. The heat capacity jump is [Formula: see text], which is lower than 1.43 expected for Bardeen-Cooper-Schrieffer (BCS) weak-coupling limit. TF-[Formula: see text]SR measurements reveal a fully gapped s-wave superconductivity with [Formula: see text], which is small compared to the BCS value of 3.56, suggesting weak-coupling superconductivity. The magnetic penetration depth, [Formula: see text], estimated from TF-[Formula: see text]SR gives [Formula: see text] nm, a superconducting carrier density [Formula: see text] carriers m-3 and a carrier effective-mass enhancement factor [Formula: see text]. ZF-[Formula: see text]SR data show no evidence for any spontaneous magnetic fields below [Formula: see text], which demonstrates that time-reversal symmetry is preserved in the superconducting state of LaIr3.

Investigation of superconducting gap structure in HfIrSi using muon spin relaxation/rotation.

We have investigated the superconducting state of HfIrSi using magnetization, specific heat, muon spin rotation and relaxation ([Formula: see text]SR) measurements. Superconductivity was observed at [Formula: see text] K in both specific heat and magnetization measurements. From an analysis of the transverse-field [Formula: see text]SR data, it is clear that the temperature variation of superfluid density is well fitted by an isotropic Bardeen-Cooper-Schrieffer (BCS) type s-wave gap structure. The superconducting carrier density [Formula: see text] m-3, the magnetic penetration depth, [Formula: see text] nm, and the effective mass, [Formula: see text], were calculated from the TF-[Formula: see text]SR data. Zero-field [Formula: see text]SR data for HfIrSi reveal the absence of any spontaneous magnetic moments below [Formula: see text], indicating that time-reversal symmetry (TRS) is preserved in the superconducting state of HfIrSi. Theoretical investigations suggest that the Hf and Ir atoms hybridize strongly along the c-axis, and that this is responsible for the strong three-dimensionality of this system which screens the Coulomb interaction. As a result, despite the presence of d-electrons in HfIrSi, these correlation effects are weakened, making the electron-phonon coupling more important.

Superconductivity and the upper critical field in the chiral noncentrosymmetric superconductor NbRh2B2.

NbRh2B2 crystallises in a chiral noncentrosymmetric structure and exhibits bulk type-II superconductivity below [Formula: see text] K. Here we show that the temperature dependence of the upper critical field deviates from the behaviour expected for both Werthamer-Helfand-Hohenberg and the Ginzburg-Landau models and that [Formula: see text] T exceeds the Pauli paramagnetic limit, [Formula: see text] T. We explore the reasons for this enhancement. Transverse-field muon spectroscopy measurements suggest that the superconducting gap is either s-wave or [Formula: see text]-wave, and the pressure dependence of [Formula: see text] reveals the superconducting gap is primarily s-wave in character. The magnetic penetration depth [Formula: see text] nm. Heat capacity measurements reveal the presence of a multigap [Formula: see text]-wave superconducting order parameter and moderate electron-phonon coupling.

Evidence for dynamic kagome ice.

The search for two-dimensional quantum spin liquids, exotic magnetic states remaining disordered down to zero temperature, has been a great challenge in frustrated magnetism over the last few decades. Recently, evidence for fractionalized excitations, called spinons, emerging from these states has been observed 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 applying a magnetic field to the pyrochlore oxide Nd2Zr2O7, which has been shown to develop three-dimensional quantum magnetic fragmentation in zero field, results in a dimensional reduction, creating a dynamic kagome ice state: the spin excitation spectrum determined by neutron scattering encompasses a flat mode with a six arm shape akin to the kagome ice structure factor, from which dispersive branches emerge.

Low temperature magnetic properties of Nd2Ru2O7.

We present magnetic susceptibility, heat capacity, and neutron diffraction measurements of polycrystalline Nd2Ru2O7 down to 0.4 K. Three anomalies in the magnetic susceptibility measurements at 146, 21 and 1.8 K are associated with an antiferromagnetic ordering of the Ru4+ moments, a weak ferromagnetic signal attributed to a canting of the Ru4+ and Nd3+ moments, and a long-range-ordering of the Nd3+ moments, respectively. The long-range order of the Nd3+ moments was observed in all the measurements, indicating that the ground state of the compound is not a spin glass. The magnetic entropy of Rln2 accumulated up to 5 K, suggests the Nd3+ has a doublet ground state. Lattice distortions accompany the transitions, as revealed by neutron diffraction measurements, and in agreement with earlier synchrotron x-ray studies. The magnetic moment of the Nd3+ ion at 0.4 K is estimated to be 1.54(2)µ B and the magnetic structure is all-in all-out as determined by our neutron diffraction measurements.

Magnetisation process in the rare earth tetraborides, NdB4 and HoB4.

A field-induced magnetisation process in the frustrated antiferromagnets is often much richer compared to the materials without competing interactions. The applied field tends to stabilise unusual spin configurations which frequently results in the appearance of magnetisation plateaux. Here we report a study into the field-induced magnetisation of the two frustrated rare earth tetraborides, HoB4 and NdB4. NdB4 shows a fractional magnetisation plateau occurring at M/M sat ≈ [Formula: see text] before saturating in a field of 33 kOe. On cooling down to 0.5 K the temperature dependent susceptibility of NdB4 shows an unconventional transition where the system returns to the zero field antiferromagnetic state from a higher-temperature ferrimagnetic state. We are able to reconstruct the magnetic phase diagram of NdB4 from the magnetisation, susceptibility and resistivity measurements for both H [Formula: see text] c and H ⊥ c. For HoB4, the most interesting behaviour is found at the lowest temperature of 0.5 K, where the field dependent magnetisation demonstrates a new fractional [Formula: see text]-magnetisation plateau. Further insight into the relations between the exchange interactions and single ion effects is gained through high-field magnetisation measurements in both HoB4 and NdB4.

Signatures of the Kondo effect in VSe2.

VSe2 is a transition metal dichaclogenide which has a charge- density wave transition that has been well studied. We report on a low-temperature upturn in the resistivity and, at temperatures below this resistivity minimum, an unusual magnetoresistance which is negative at low fields and positive at higher fields, in single crystals of VSe2. The negative magnetoresistance has a parabolic dependence on the magnetic field and shows little angular dependence. The magnetoresistance at temperatures above the resistivity minimum is always positive. We interpret these results as signatures of the Kondo effect in VSe2. An upturn in the susceptibility indicates the presence of interlayer V ions which can provide the localized magnetic moments required for scattering the conduction electrons in the Kondo effect. The low-temperature behaviour of the heat capacity, including a high value of γ, along with a deviation from a Curie-Weiss law observed in the low-temperature magnetic susceptibility, are consistent with the presence of magnetic interactions between the paramagnetic interlayer V ions and a Kondo screening of these V moments.

Colossal Terahertz Magnetoresistance at Room Temperature in Epitaxial La0.7Sr0.3MnO3 Nanocomposites and Single-Phase Thin Films.

Colossal magnetoresistance (CMR) is demonstrated at terahertz (THz) frequencies by using terahertz time-domain magnetospectroscopy to examine vertically aligned nanocomposites (VANs) and planar thin films of La0.7Sr0.3MnO3. At the Curie temperature (room temperature), the THz conductivity of the VAN was dramatically enhanced by over 2 orders of magnitude under the application of a magnetic field with a non-Drude THz conductivity that increased with frequency. The direct current (dc) CMR of the VAN is controlled by extrinsic magnetotransport mechanisms such as spin-polarized tunneling between nanograins. In contrast, we find that THz CMR is dominated by intrinsic, intragrain transport: the mean free path was smaller than the nanocolumn size, and the planar thin-film exhibited similar THz CMR to the VAN. Surprisingly, the observed colossal THz magnetoresistance suggests that the magnetoresistance can be large for alternating current motion on nanometer length scales, even when the magnetoresistance is negligible on the macroscopic length scales probed by dc transport. This suggests that colossal magnetoresistance at THz frequencies may find use in nanoelectronics and in THz optical components controlled by magnetic fields. The VAN can be scaled in thickness while retaining a high structural quality and offers a larger THz CMR at room temperature than the planar film.

Robust singlet dimers with fragile ordering in two-dimensional honeycomb lattice of Li2RuO3.

When an electronic system has strong correlations and a large spin-orbit interaction, it often exhibits a plethora of mutually competing quantum phases. How a particular quantum ground state is selected out of several possibilities is a very interesting question. However, equally fascinating is how such a quantum entangled state breaks up due to perturbation. This important question has relevance in very diverse fields of science from strongly correlated electron physics to quantum information. Here we report that a quantum entangled dimerized state or valence bond crystal (VBC) phase of Li2RuO3 shows nontrivial doping dependence as we perturb the Ru honeycomb lattice by replacing Ru with Li. Through extensive experimental studies, we demonstrate that the VBC phase melts into a valence bond liquid phase of the RVB (resonating valence bond) type. This system offers an interesting playground where one can test and refine our current understanding of the quantum competing phases in a single compound.

Structure and magnetism in Cr-embedded Co nanoparticles.

We present the results of an investigation into the atomic structure and magnetism of 2 nm diameter Co nanoparticles embedded in an antiferromagnetic Cr matrix. The nanocomposite films used in this study were prepared by co-deposition directly from the gas phase, using a gas aggregation source for the Co nanoparticles and a molecular beam epitaxy (MBE) source for the Cr matrix material. Co K and Cr K edge extended x-ray absorption fine structure (EXAFS) experiments were performed in order to investigate atomic structure in the embedded nanoparticles and matrix respectively, while magnetism was investigated by means of a vibrating sample magnetometer. The atomic structure type of the Co nanoparticles is the same as that of the Cr matrix (bcc) although with a degree of disorder. The net Co moment per atom in the Co/Cr nanocomposite films is significantly reduced from the value for bulk Co, and decreases as the proportion of Co nanoparticles in the film is decreased; for the sample with the most dilute concentration of Co nanoparticles (4.9% by volume), the net Co moment was 0.25 µ B/atom. After field cooling to below 30 K all samples showed an exchange bias, which was largest for the most dilute sample. Both the structural and magnetic results point towards a degree of alloying at the nanoparticle/matrix interface, leading to a core/shell structure in the embedded nanoparticles consisting of an antiferromagnetic CoCr alloy shell surrounding a reduced ferromagnetic Co core.

Fluctuations and All-In-All-Out Ordering in Dipole-Octupole Nd(2)Zr(2)O(7).

By means of neutron scattering and magnetization measurements down to 90 mK, we determine the magnetic ground state of the spin-ice candidate Nd(2)Zr(2)O(7). We show that, despite ferromagnetic interactions, Nd(2)Zr(2)O(7) undergoes a transition around 285 mK towards an all-in-all-out antiferromagnetic state, with a strongly reduced ordered magnetic moment. We establish the (H,T) phase diagram in the three directions of the applied field and reveal a metamagnetic transition around 0.1 T, associated with an unexpected shape of the magnetization curves. We propose that this behavior results from the peculiar nature of the Nd^{3+} doublet, a dipolar-octupolar doublet, different from the standard Kramers doublet studied to date, thus revealing the importance of multipolar correlations in the properties of pyrochlore oxides.

Effects of rare-earth size on the electronic structure of La1−xLuxVO3.

The electronic structure of La(1-x)Lu(x)VO(3)(x = 0, 0.2, 0.6 and 1) single crystals has been investigated using soft x-ray absorption spectroscopy, soft x-ray emission spectroscopy, and resonant soft x-ray inelastic scattering to study the effects of rare-earth size. The x-ray absorption and emission spectra at the O K-edge present a progressive evolution with R-site cation, in agreement with local spin density approximation calculations. This evolution with R, together with the temperature dependence of the O K-edge spectra, is attributed to changes in the crystal structure of La(1-x)Lu(x)VO(3). The crystal-field dd. excitations probed by resonant inelastic x-ray scattering at the V L(3)-edge exhibit an increase in energy and enhanced intensity with the decrease of R-site ionic radius, which is mainly attributed to the increased tilting magnitude of the VO(6) octahedra. Upon cooling to ~95 K, the dd* excitations are prominently enhanced in relative Intensity, in agreement with the formation of the Jahn.Teller distortion int he orbital ordering phase. Additionally, the dd* transitions of the mixed compounds are noticeably suppressed with respect to those of the pure compounds, possibly owing to the formation of C-type orbital ordering induced by large R-site size variances.

Structural, optical and vibrational properties of self-assembled Pbn+1(Ti1-x Fex)nO(3n+1)-δ Ruddlesden-Popper superstructures.

Bulk crystals and thin films of PbTi(1-x)FexO3(-δ) (PTFO) are multiferroic, exhibiting ferroelectricity and ferromagnetism at room temperature. Here we report that the Ruddlesden-Popper phase Pbn+1(Ti(1-x)Fex)nO3(n+1)-δ forms spontaneously during pulsed laser deposition of PTFO on LaAlO3 substrates. High-resolution transmission electron microscopy, x-ray diffraction and x-ray photoemission spectroscopy were utilised to perform a structural and compositional analysis, demonstrating that n ≃ 8 and x ≃ 0.5. The complex dielectric function of the films was determined from far-infrared to ultraviolet energies using a combination of terahertz time-domain spectroscopy, Fourier transform spectroscopy, and spectroscopic ellipsometry. The simultaneous Raman and infrared activity of phonon modes and the observation of second harmonic generation establishes a non-centrosymmetric point group for Pbn+1(Ti0.5Fe0.5)nO3(n+1)-δ, a prerequisite for (but not proof of) ferroelectricity. No evidence of macroscopic ferromagnetism was found in SQUID magnetometry. The ultrafast optical response exhibited coherent magnon oscillations compatible with local magnetic order, and additionally was used to study photocarrier cooling on picosecond timescales. An optical gap smaller than that of BiFeO3 and long photocarrier lifetimes may make this system interesting as a ferroelectric photovoltaic.

Unconventional Superconductivity in La(7)Ir(3) Revealed by Muon Spin Relaxation: Introducing a New Family of Noncentrosymmetric Superconductor That Breaks Time-Reversal Symmetry.

The superconductivity of the noncentrosymmetric compound La(7)Ir(3) is investigated using muon spin rotation and relaxation. Zero-field measurements reveal the presence of spontaneous static or quasistatic magnetic fields below the superconducting transition temperature T(c)=2.25 K-a clear indication that the superconducting state breaks time-reversal symmetry. Furthermore, transverse-field rotation measurements suggest that the superconducting gap is isotropic and that the pairing symmetry of the superconducting electrons is predominantly s wave with an enhanced binding strength. The results indicate that the superconductivity in La(7)Ir(3) may be unconventional and paves the way for further studies of this family of materials.

Magnetic susceptibility and heat capacity measurements of single crystal TbMnO3.

Measurements of the magnetic susceptibility χ and heat capacity C on single crystals of the multiferroic TbMnO3 are presented. A non-magnetic isostructural compound, LaGaO3, was used to isolate the magnetic component of the heat capacity. An anisotropic magnetic susceptibility, deviations from Curie-Weiss behaviour and a significant magnetic entropy above the antiferromagnetic ordering temperature TN1 = 41 K are attributed to a combination of crystal-field effects and short-range order between the Mn moments. Heat capacity in a magnetic field applied along the a axis confirms the saturation of Tb(3+) moments in 90 kOe. A hyperfine contribution from the Tb and Mn nuclear moments that may be convolved with a contribution from low-lying Tb crystal-field levels leads to a low-temperature rise in C(T)/T.

Detection of time-reversal symmetry breaking in the noncentrosymmetric superconductor Re6Zr using muon-spin spectroscopy.

We have investigated the superconducting state of the noncentrosymmetric compound Re6Zr using magnetization, heat capacity, and muon-spin relaxation or rotation (µSR) measurements. Re6Zr has a superconducting transition temperature, Tc=6.75±0.05 K. Transverse-field µSR experiments, used to probe the superfluid density, suggest an s-wave character for the superconducting gap. However, zero and longitudinal-field µSR data reveal the presence of spontaneous static magnetic fields below Tc indicating that time-reversal symmetry is broken in the superconducting state and an unconventional pairing mechanism. An analysis of the pairing symmetries identifies the ground states compatible with time-reversal symmetry breaking.

Large, high quality single-crystals of the new Topological Kondo Insulator, SmB6.

SmB6 has recently been predicted to be a Topological Kondo Insulator, the first strongly correlated heavy fermion material to exhibit topological surface states. High quality crystals are necessary to investigate the topological properties of this material. Single crystal growth of the rare earth hexaboride, SmB6, has been carried out by the floating zone technique using a high power xenon arc lamp image furnace. Large, high quality single-crystals are obtained by this technique. The crystals produced by the floating zone technique are free of contamination from flux materials and have been characterised by resistivity and magnetisation measurements. These crystals are ideally suited for the investigation of both the surface and bulk properties of SmB6.