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A large anomalous Hall effect (AHE) has recently been observed in the intercalated transition metal dichalcogenide (TMDC) Co$_{1/3}$NbS$_{2}$ below a known magnetic phase transition at $T_N$ = 29 K. The spins in this material are widely believed to order in a highly symmetric collinear antiferromagnetic configuration, causing extensive debate about how reports of an AHE can be reconciled with such a state. In this article, we address this controversy by presenting new neutron diffraction data on single crystals of Co$_{1/3}$NbS$_{2}$ and an analysis that implies that moments in this material order into a non-collinear configuration, but one that maintains the same refelction symmetries as the collinear phase. We present new transport and magneto-optic Kerr measurements which show that AHE signatures persist below $T_N$ to temperatures as low as $T$ = 5 K and firmly associate them with the long-range antiferromagnetic order. Finally, we show that these AHE signatures can be quantitatively reproduced by density functional theory (DFT) calculations based on the lattice and spin state determined with neutron diffraction. These combined findings establishes the veracity of the 'crystal Hall effect' picture, which shows how such effects can emerge from the shape of magnetic orbitals in compounds containing chiral lattice symmetry regardless of the symmetry of the ordered spin configuration. These results illuminate a new path for the discovery of anomalous Hall materials and motivate a targeted study of the transport properties of intercalated TMDCs and other compounds containing antiferromagnetic order and chiral lattice symmetry., Comment: 13 pages, 7 figures

Iridates with the 5$d^4$ electronic configuration have attracted recent interest due to reports of magnetically-ordered ground states despite longstanding expectations that their strong spin-orbit coupling would generate a $J = 0$ electronic ground state for each Ir$^{5+}$ ion. The major focus of prior research has been on the double perovskite iridates Ba$_2$YIrO$_6$ and Sr$_2$YIrO$_6$, where the nature of the ground states (i.e. ordered vs non-magnetic) is still controversial. Here we present neutron powder diffraction, high energy resolution fluorescence detected x-ray absorption spectroscopy (HERFD-XAS), resonant inelastic x-ray scattering (RIXS), magnetic susceptibility, and muon spin relaxation data on the related double perovskite iridates Ba$_2$LuIrO$_6$, Sr$_2$LuIrO$_6$, Ba$_2$ScIrO$_6$, and Sr$_2$ScIrO$_6$ that enable us to gain a general understanding of the electronic and magnetic properties for this family of materials. Our HERFD-XAS and RIXS measurements establish $J = 0$ electronic ground states for the Ir$^{5+}$ ions in all cases, with similar values for Hund's coupling $J_{\rm H}$ and the spin-orbit coupling constant $\lambda_{\rm SOC}$. Our bulk susceptibility and muon spin relaxation data find no evidence for long-range magnetic order or spin freezing, but they do reveal weak magnetic signals that are consistent with extrinsic local moments. Our results indicate that the large $\lambda_{\rm SOC}$ is the key driving force behind the electronic and magnetic ground states realized in the 5$d^4$ double perovskite iridates, which agrees well with conventional wisdom., Comment: 13 pages, 7 figures, accepted for publication by PRM

The manipulation of mesoscale domain wall phenomena has emerged as a powerful strategy for designing ferroelectric responses in functional devices, but its full potential has not yet been realized in the field of magnetism. We show that mechanically strained samples of Mn$_3$O$_4$ and MnV$_2$O$_4$ exhibit a stripe-like patterning of the bulk magnetization below known magnetostructural transitions, similar to the structural domains reported in ferroelectric materials. Building off our previous magnetic force microscopy data, we use small angle neutron scattering to show that these patterns extend to the bulk, and demonstrate an ability to manipulate the domain walls via applied magnetic field and mechanical stress. We then connect these domains back to the anomalously large magnetoelastic and magnetodielectric response functions reported in these materials, directly correlating local and macroscopic measurements on the same crystals., Comment: 19 pages, 13 figures

Heavy transition metal magnets with $J_{\rm eff}$ $=$ 1/2 electronic ground states have attracted recent interest due to their penchant for hosting new classes of quantum spin liquids and superconductors. Unfortunately, model systems with ideal $J_{\rm eff}$ $=$ 1/2 states are scarce due to the importance of non-cubic local distortions in most candidate materials. In this work, we identify a family of iridium halide systems [i.e. K$_2$IrCl$_6$, K$_2$IrBr$_6$, (NH$_4$)$_2$IrCl$_6$, and Na$_2$IrCl$_6 \cdotp $ 6(H$_2$O)] with Ir$^{4+}$ electronic ground states in extremely close proximity to the ideal $J_{\rm eff}$ $=$ 1/2 limit, despite a variation in the low-temperature global crystal structures. We also find ordered magnetic ground states for the three anhydrous systems, with single crystal neutron diffraction on K$_2$IrBr$_6$ revealing Type-I antiferromagnetism. This spin configuration is consistent with expectations for significant Kitaev exchange in a face-centered-cubic magnet., Comment: 14 pages, 9 figures

Charge density wave (CDW) correlations are prevalent in all copper-oxide superconductors. While CDWs in conventional metals are driven by coupling between lattice vibrations and electrons, the role of the electron-phonon coupling (EPC) in cuprate CDWs is strongly debated. Using Cu $L_3$ edge resonant inelastic x-ray scattering (RIXS), we study the CDW and Cu-O bond-stretching phonons in the stripe-ordered cuprate La$_{1.8-x}$Eu$_{0.2}$Sr$_{x}$CuO$_{4+\delta}$. We investigate the interplay between charge order and EPC as a function of doping and temperature, and find that the EPC is enhanced in a narrow momentum region around the CDW wave vector. By detuning the incident photon energy from the absorption resonance, we extract an EPC matrix element at the CDW wave vector of $M\simeq$ 0.36 eV, which decreases to $M\simeq$ 0.30 eV at high temperature in the absence of the CDW. Our results suggest a feedback mechanism in which the CDW enhances the EPC which, in turn, further stabilizes the CDW., Comment: 5 pages, 4 figures

The symmetry of local moments plays a defining role in the nature of exotic grounds states stabilized in frustrated magnetic materials. We present inelastic neutron scattering (INS) measurements of the crystal electric field (CEF) excitations in the family of compounds MgRE$_2$Se$_4$ (RE $\in$ $\{$Ho, Tm, Er and Yb$\}$). These compounds form in the spinel structure, with the rare earth ions comprising a highly frustrated pyrochlore sublattice. Within the symmetry constraints of this lattice, we fit both the energies and intensities of observed modes in the INS spectra to determine the most likely CEF Hamiltonian for each material and comment on the ground state wavefunctions in the local electron picture. In this way, we experimentally confirm MgTm$_2$Se$_4$ has a non-magnetic ground state, and MgYb$_2$Se$_4$ has effective $S=\frac{1}{2}$ spins with $g_\parallel = 5.188(79)$ and $g_\perp = 0.923(85)~\mu_B$. The spectrum of MgHo$_2$Se$_4$ indicates a ground state doublet containing Ising spins with $g_\parallel = 2.72(46)$, though low-lying CEF levels are also seen at thermally accessible energies $\delta_E = 0.591(36)$, 0.945(30) and 2.88(7)~meV, which can complicate interpretation. These results are used to comment on measured magnetization data of all compounds, and are compared to published results on the material MgEr$_2$Se$_4$., Comment: 13 pages, 7 figures

Quantum magnets with significant bond-directional Ising interactions, so-called Kitaev materials, have attracted tremendous attention recently in the search for exotic spin liquid states. Here we present a comprehensive set of measurements that enables us to investigate the crystal structures, Ir$^{4+}$ single ion properties, and magnetic ground states of the double perovskite iridates La$_2B$IrO$_6$ ($B$ $=$ Mg, Zn) and $A_2$CeIrO$_6$ ($A$ $=$ Ba, Sr) with a large nearest neighbor distance $>$ 5 Angstroms between Ir$^{4+}$ ions. Our neutron powder diffraction data on Ba$_2$CeIrO$_6$ can be refined in the cubic space group Fm$\bar{3}$m, while the other three systems are characterized by weak monoclinic structural distortions. Despite the variance in the non-cubic crystal field experienced by the Ir$^{4+}$ ions in these materials, X-ray absorption spectroscopy and resonant inelastic x-ray scattering are consistent with $J_{\rm eff}$ $=$ 1/2 moments in all cases. Furthermore, neutron scattering and resonant magnetic x-ray scattering show that these systems host A-type antiferromagnetic order. These electronic and magnetic ground states are consistent with expectations for face-centered-cubic magnets with significant antiferromagnetic Kitaev exchange, which indicates that spacing magnetic ions far apart may be a promising design principle for uncovering additional Kitaev materials., Comment: 12 pages, 7 figures

Controlling multiferroic behavior in materials will enable the development of a wide variety of technological applications. However, the exact mechanisms driving multiferroic behavior are not well understood in most materials. Two such materials are the spinels MnV2O4 and Mn3O4, where mechanical strain is thought to play a role in determining magnetic behavior. Bulk studies of MnV2O4 have yielded conflicting and inconclusive results, due in part to the presence of mesoscale magnetic inhomogeneity, which complicates the interpretation of bulk measurements. To study the sub-micron-scale magnetic properties of Mn-based spinel materials, we performed magnetic force microscopy (MFM) on MnV2O4 samples subject to different levels of mechanical strain. We also used a crystal grain mapping technique to perform spatially registered MFM on Mn3O4. These local investigations revealed 100-nm-scale "stripe" modulations in the magnetic structure of both materials. In MnV2O4, the magnetization of these stripes is estimated to be Mz $\approx$ 105 A/m, which is on the order of the saturation magnetization reported previously. Cooling in a strong magnetic field eliminated the stripe patterning only in the low-strain sample of MnV2O4. The discovery of nanoscale magnetostructural inhomogeneity that is highly susceptible to magnetic field control in these materials necessitates both a revision of theoretical proposals and a reinterpretation of experimental data regarding the low-temperature phases and magnetic-field-tunable properties of these Mn-based spinels., Comment: 23 pages, 8 figures, To be published in Physical Review Materials

In frustrated spinel antiferromagnets, dilution with non-magnetic ions can be a powerful strategy for probing unconventional spin states or uncovering interesting phenomena. Here, we present X-ray, neutron scattering and thermodynamic studies of the effects of magnetic dilution of the tetragonally-distorted A-site spinel antiferromagnet, CuRh$_2$O$_4$, with non-magnetic Zn$^{2+}$ ions. Our data confirm the helical spin order recently identified at low-temperatures in this material, and further demonstrate a systematic suppression of the associated N\'eel temperature with increasing site dilution towards a continuous transition with critical doping of $x_{spin} \sim 0.44$. Interestingly, this critical doping is demonstrably distinct from a second structural critical point at $x_{JT} \sim 0.6$, which is consistent with the suppression of orbital order on the A-site through a classical percolative mechanism. This anomalously low value for $x_{spin}$ is confirmed via multiple measurements, and is inconsistent with predictions of classical percolation theory, suggesting that the spin transition in this material is driven by an enhancement of pre-existing spin fluctuations with weak dilution., Comment: 9 pages, 5 figures

In spin ice research, small variations in structure or interactions drive a multitude of different behaviors, yet the collection of known materials relies heavily on the `227' pyrochlore structure. Here, we present thermodynamic, structural and inelastic neutron scattering data on a new spin-ice material, MgEr$_2$Se$_4$, which contributes to the relatively under-explored family of rare-earth spinel chalcogenides. X-ray and neutron diffraction confirm a normal spinel structure, and places Er$^{3+}$ moments on an ideal pyrochlore sublattice. Measurement of crystal electric field excitations with inelastic neutron scattering confirms that the moments have perfect Ising character, and further identifies the ground state Kramers doublet as having dipolar-octupolar form with a significant multipolar character. Heat capacity and magnetic neutron diffuse scattering have ice-like features, but are inconsistent with Monte Carlo simulations of the nearest-neighbor and next-nearest-neighbor dipolar spin-ice (DSI) models. A significant remnant entropy is observed as $T\rightarrow0$~K, but again falls short of the full Pauling expectation for DSI, unless significant disorder is added. We show that these observations are fully in-line with what is recently reported for CdEr$_2$Se$_4$, and point to the importance of quantum fluctuations in these materials., Comment: 12 pages with 12 figures, including appendix. Changes since last revision include, new monte carlo simulations fitting to the neutron powder diffraction data, update of crystal field parameter fitting method to find error bars, update of magnetization calculation for higher accuracy at high field, and numerous updates to wording for better clarity and fixing spelling and formatting issues

The A-site spinel material, CoAl2O4, is a physical realization of the frustrated diamond-lattice antiferromagnet, a model in which is predicted to contain unique incommensurate or `spin-spiral liquid' ground states. Our previous single-crystal neutron scattering study instead classified it as a `kinetically-inhibited' antiferromagnet, where the long ranged correlations of a collinear Neel ground state are blocked by the freezing of domain wall motion below a first-order phase transition at T* = 6.5 K. The current paper expands on our original results in several important ways. New elastic and inelastic neutron measurements are presented that show our initial conclusions are affected by neither the sample measured nor the instrument resolution, while measurements to temperatures as low as T = 250 mK limit the possible role being played by low-lying thermal excitations. Polarized diffuse neutron measurements confirm reports of short-range antiferromagnetic correlations and diffuse streaks of scattering, but major diffuse features are explained as signatures of overlapping critical correlations between neighboring Brillouin zones. Finally, and critically, this paper presents detailed elastic and inelastic measurements of magnetic correlations in a single-crystal of MnAl2O4, which acts as an unfrustrated analogue to CoAl2O4. The unfrustrated material is shown to have a classical continuous phase transition to Neel order at T_N = 39 K, with collective spinwave excitations and Lorentzian-like critical correlations which diverge at the transition. Direct comparison between the two compounds indicates that CoAl2O4 is unique, not in the nature of high-temperature diffuse correlations, but rather in the nature of the frozen state below T*. The higher level of cation inversion in the MnAl2O4 sample indicates that this novel behavior is primarily an effect of greater next-nearest-neighbor exchange., Comment: 13 pages, 8 figures, acccepted for publication in Physical Review B

The ferrimagnetic spinel Mn3O4 exhibits large and anisotropic changes in electronic and structural properties in response to an applied magnetic field. These changes are thought to result from the field-dependent tuning---via strong spin-lattice coupling---between two nearly degenerate magnetostructural phases. Recent variable-magnetic-field studies of Mn3O4 have been performed on melt-grown crystals, which can exhibit twin domains due to a Jahn-Teller structural transition below the melting temperature. Because of the near degeneracy of the magnetostructural phases, however, strain associated with the twin domains likely affects the magnetic responses of Mn3O4. In this report, we present a variable-magnetic-field Raman scattering study of untwinned Mn3O4 crystals grown out of a flux below the Jahn-Teller structural transition. We measure distinct q = 0 magnetic and vibrational excitation spectra for each isolated magnetostructural phase of untwinned Mn3O4 crystals and determine the symmetries of the observed excitations. We determine how the magnetostructural phase mixture changes in response to magnetic fields applied in the magnetic easy plane. Lastly, by comparing results on flux- and melt-grown Mn3O4 crystals, we show that the intrinsic mixture of the two magnetostructural phases is indeed strongly influenced by the presence of twin domains.

The ferrimagnetic spinel $\mathrm{CoV_2O_4}$ has been a topic of intense recent interest, both as a frustrated insulator with unquenched orbital degeneracy and as a near-itinerant magnet which can be driven metallic with moderate applied pressure. Here, we report on our recent neutron diffraction and inelastic scattering measurements on powders with minimal cation site disorder. Our main new result is the identification of a weak ($\frac{\Delta a}{a} \sim 10^{-4}$), first order structural phase transition at $T^*$ = 90 K, the same temperature where spin canting was seen in recent single crystal measurements. This transition is characterized by a short-range distortion of oxygen octahedral positions, and inelastic data further establish a weak $\Delta\sim 1.25 meV$ spin gap at low temperature. Together, these findings provide strong support for the local orbital picture and the existence of an orbital glass state at temperatures below $T^*$., Comment: 8 pages, 5 figures, To be published in Physical Review B

We used low-energy, momentum-resolved inelastic electron scattering to study surface collective modes of the three-dimensional topological insulators Bi$_2$Se$_3$ and Bi$_{0.5}$Sb$_{1.5}$Te$_{3-x}$Se$_{x}$. Our goal was to identify the "spin plasmon" predicted by Raghu and co-workers [S. Raghu, et al., Phys. Rev. Lett. 104, 116401 (2010)]. Instead, we found that the primary collective mode is a surface plasmon arising from the bulk, free carrers in these materials. This excitation dominates the spectral weight in the bosonic function of the surface, $\chi "(\textbf{q},\omega)$, at THz energy scales, and is the most likely origin of a quasiparticle dispersion kink observed in previous photoemission experiments. Our study suggests that the spin plasmon may mix with this other surface mode, calling for a more nuanced understanding of optical experiments in which the spin plasmon is reported to play a role., Comment: 5 pages, 4 figures

The ferrimagnetic spinels MnB2O4 (B = Mn,V) exhibit a similar series of closely spaced magnetic and structural phase transitions at low temperatures, reflecting both magnetic frustration and a strong coupling between the spin and lattice degrees of freedom. Careful studies of excitations in MnB2O4 (B = Mn,V), and the evolution of these excitations with temperature, are important for obtaining a microscopic description of the role that magnetic excitations and spin-lattice coupling play in the low temperature phase transitions of these materials. We report an inelastic light (Raman) scattering study of the temperature and magnetic field dependences of one- and two-magnon excitations in MnV2O4 and Mn3O4. We observe a pair of q=0 one-magnon modes at 74 cm^{-1} and 81 cm^{-1} in MnV2O4, which is in contrast with the single 80 cm^{-1} q=0 magnon that has been reported for MnV2O4 based on previous neutron scattering measurements and spin wave calculations. Additionally, we find that the two-magnon energy of MnV2O4 decreases ("softens") with decreasing temperature below T_{N}, which we attribute to strong coupling between magnetic and vibrational excitations near the zone boundary., Comment: 7 pages, 4 figures

Superconductivity evolves as functions of pressure or doping from charge-ordered phases in a variety of strongly correlated systems, suggesting that there may be universal characteristics associated with the competition between superconductivity and charge order in these materials. We present an inelastic light (Raman) scattering study of the structural changes that precede the pressure-tuned charge-density-wave (CDW) to superconductor transition in one such system, ZrTe3. In certain phonon bands, we observe dramatic linewidth reductions that accompany CDW formation, indicating that these phonons couple strongly to the electronic degrees of freedom associated with the CDW. The same phonon bands, which represent internal vibrations of ZrTe3 prismatic chains, are suppressed at pressures above ~10 kbar, indicating a loss of long-range order within the chains, specifically amongst intrachain Zr-Te bonds. These results suggest a distinct structural mechanism for the observed pressure-induced suppression of CDW formation and provide insights into the origin of pressure-induced superconductivity in ZrTe3., Comment: 6 pages, 5 figures

We report temperature-dependent transport and x-ray diffraction measurements of the influence of Ti hole doping on the charge density wave (CDW) in 1T-Ta(1-x)Ti(x)S(2). Confirming past studies, we find that even trace impurities eliminate the low-temperature commensurate (C) phase in this system. Surprisingly, the magnitude of the in-plane component of the CDW wave vector in the nearly commensurate (NC) phase does not change significantly with Ti concentration, as might be expected from a changing Fermi surface volume. Instead, the angle of the CDW in the basal plane rotates, from 11.9 deg at x=0 to 16.4 deg at x=0.12. Ti substitution also leads to an extended region of coexistence between incommensurate (IC) and NC phases, indicating heterogeneous nucleation near the transition. Finally, we explain a resistive anomaly originally observed by DiSalvo [F. J. DiSalvo, et al., Phys. Rev. B {\bf 12}, 2220 (1975)] as arising from pinning of the CDW on the crystal lattice. Our study highlights the importance of commensuration effects in the NC phase, particularly at x ~ 0.08.

The spinel vanadates have become a model family for exploring orbital order on the frustrated pyrochlore lattice, and recent debate has focused on the symmetry of local crystal fields at the cation sites. Here, we present neutron scattering measurements of the magnetic excitation spectrum in $\mathrm{FeV_2O_4}$, a recent example of a ferrimagnetic spinel vanadate which is available in single crystal form. We report the existence of two emergent magnon modes at low temperatures, which draw strong parallels with the closely related material, $\mathrm{MnV_2O_4}$. We were able to reproduce the essential elements of both the magnetic ordering pattern and the dispersion of the inelastic modes with semi- classical spin wave calculations, using a minimal model that implies a sizeable single-ion anisotropy on the vanadium sublattice. Taking into account the direction of ordered spins, we associate this anisotropy with the large trigonal distortion of $\mathrm{VO_6}$ octahedra, previously observed via neutron powder diffraction measurements. We further report on the spin gap, which is an order-of-magnitude larger than that observed in $\mathrm{MnV_2O_4}$. By looking at the overall temperature dependence, we were able to show that the gap magnitude is largely associated with the ferro-orbital order known to exist on the iron sublattice, but the contribution to the gap from the vanadium sublattice is in fact comparable to what is reported in the Mn compound. This reinforces the conclusion that the spin canting transition is associated with the ordering of vanadium orbitals in this system, and closer analysis indicates closely related physics underlying orbital transitions in $\mathrm{FeV_2O_4}$ and $\mathrm{MnV_2O_4}$., Comment: 8 pages, 6 figures, includes supplementary figure; accepted for publication in Physical Review B

Superconductivity (SC) in so-called "unconventional superconductors" is nearly always found in the vicinity of another ordered state, such as antiferromagnetism, charge density wave (CDW), or stripe order. This suggests a fundamental connection between SC and fluctuations in some other order parameter. To better understand this connection, we used high-pressure x-ray scattering to directly study the CDW order in the layered dichalcogenide TiSe2, which was previously shown to exhibit SC when the CDW is suppressed by pressure [1] or intercalation of Cu atoms [2]. We succeeded in suppressing the CDW fully to zero temperature, establishing for the first time the existence of a quantum critical point (QCP) at Pc = 5.1 +/- 0.2 GPa, which is more than 1 GPa beyond the end of the SC region. Unexpectedly, at P = 3 GPa we observed a reentrant, weakly first order, incommensurate phase, indicating the presence of a Lifshitz tricritical point somewhere above the superconducting dome. Our study suggests that SC in TiSe2 may not be connected to the QCP itself, but to the formation of CDW domain walls., Comment: 10 pages, 3 figures

The vibrational excitations of crystalline solids corresponding to acoustic or optic one phonon modes appear as sharp features in measurements such as neutron spectroscopy. In contrast, many-phonon excitations generally produce a complicated, weak, and featureless response. Here we present time-of-flight neutron scattering measurements for the binary solid uranium nitride (UN), showing well-defined, equally-spaced, high energy vibrational modes in addition to the usual phonons. The spectrum is that of a single atom, isotropic quantum harmonic oscillator and characterizes independent motions of light nitrogen atoms, each found in an octahedral cage of heavy uranium atoms. This is an unexpected and beautiful experimental realization of one of the fundamental, exactly-solvable problems in quantum mechanics. There are also practical implications, as the oscillator modes must be accounted for in the design of generation IV nuclear reactors that plan to use UN as a fuel., Comment: 25 pages, 10 figures, submitted to Nature Communications, supplementary information added

We present a neutron diffraction study of FeV2O4, which is rare in exhibiting spin and orbital degrees of freedom on both cation sublattices of the spinel structure. Our data confirm the existence of three structural phase transitions previously identified with x-ray powder diffraction, and reveal that the lower two transitions are associated with sequential collinear and canted ferrimagnetic transitions involving both cation sites. Through consideration of local crystal and spin symmetry, we further conclude that Fe2+ cations are ferro-orbitally ordered below 135K and V3+ orbitals order at 60K in accordance with predictions for vanadium spinels with large trigonal distortions and strong spin-orbit coupling. Intriguingly, the direction of ordered vanadium spins at low temperatures obey `ice rules' more commonly associated with the frustrated rare-earth pyrochlore systems., Comment: 10 pages, 9 figures, including Supplemental Material

Recent studies have reported the existence of an epitaxially-stabilized tetragonal-like ('T-like') monoclinic phase in BiFeO3 thin-films with high levels of compressive strain. While their structural and ferroelectric properties are different than those of rhombohedral-like ('R-like') films with lower levels of strain, little information exists on magnetic properties. Here, we report a detailed neutron scattering study of a nearly phase-pure film of T-like BiFeO3. By tracking the temperature dependence and relative intensity of several superstructure peaks in the reciprocal lattice cell, we confirm antiferromagnetism with largely G-type character and TN = 324 K, significantly below a structural phase transition at 375 K, contrary to previous reports. Evidence for a second transition, possibly a minority magnetic phase with C-type character is also reported with TN = 260 K. The co-existence of the two magnetic phases in T-like BiFeO3 and the difference in ordering temperatures between R-like and T-like systems is explained through simple Fe-O-Fe bond distance considerations., Comment: 9 pages, 7 figures. Slight modifications to introductory text and presentation of data. Supplementary Material section added

Frustrated magnetic systems exhibit highly degenerate ground states and strong fluctuations, often leading to new physics. An intriguing example of current interest is the antiferromagnet on a diamond lattice, realized physically in A-site spinel materials. This is a prototypical system in three dimensions where frustration arises from competing interactions rather than purely geometric constraints, and theory suggests the possibility of unusual magnetic order at low temperature. Here we present a comprehensive single-crystal neutron scattering study of CoAl2O4, a highly frustrated A-site spinel. We observe strong diffuse scattering that peaks at wavevectors associated with Neel ordering. Below the temperature T*=6.5 K, there is a dramatic change in the elastic scattering lineshape accompanied by the emergence of well-defined spin-wave excitations. T* had previously been associated with the onset of glassy behavior. Our new results suggest instead that T* signifies a first-order phase transition, but with true long-range order inhibited by the kinetic freezing of domain walls. This scenario might be expected to occur widely in frustrated systems containing first-order phase transitions and is a natural explanation for existing reports of anomalous glassy behavior in other materials., Comment: 40 pages, 9 figures, Introduction and discussion altered and expanded. Additional section and figure added to Supplementary Information

Impurity-induced magnetic order has been observed in many quasi-1D systems including doped variants of the spin-Peierls system CuGeO3. TiOCl is another quasi-1D quantum magnet with a spin-Peierls ground state, and the magnetic Ti sites of this system can be doped with non-magnetic Sc. To investigate the role of non-magnetic impurities in this system, we have performed both zero field and longitudinal field muSR experiments on polycrystalline Ti1-xScxOCl samples with x = 0, 0.01, and 0.03. We verified that TiOCl has a non-magnetic ground state, and we found no evidence for spin freezing or magnetic ordering in the lightly-doped Sc samples down to 1.7 K. Our results instead suggest that these systems remain non-magnetic up to the x = 0.03 Sc doping level., Comment: 5 pages, 4 figures

$LiHo_xY_{1-x}F_4$ is an insulating system where the magnetic Ho$^{3+}$ ions have an Ising character, and interact mainly through magnetic dipolar fields. We used the muon spin relaxation technique to study the nature of the ground state for samples with x=0.25, 0.12, 0.08, 0.045 and 0.018. In contrast with some previous works, we have not found any signature of canonical spin glass behavior down to $\approx$15mK. Instead, below $\approx$300mK we observed dynamic magnetism characterized by a single correlation time with a temperature independent fluctuation rate. We observed that this low temperature fluctuation rate increases with x up to 0.08, above which it levels off. The 300mK energy scale corresponds to the Ho3+ hyperfine interaction strength, suggesting that the hyperfine interaction may be intimately involved with the spin dynamics in this system.

The nature of the superconducting state in the recently discovered Fe-based superconductors1-3 is the subject of intense scrutiny. Neutron scattering investigations have already elucidated a strong correlation between magnetism and superconductivity in the form of a spin resonance in the magnetic excitation spectrum4-7. A central unanswered question concerns the nature of the normal state spin fluctuations which may be responsible for the pairing mechanism. Here we show inelastic neutron scattering measurements of Fe1.04Te0.73Se0.27, not superconducting in bulk, and FeTe0.51Se0.49, a bulk superconductor. These measurements demonstrate that the spin fluctuation spectrum is dominated by two-dimensional incommensurate excitations near the (1/2,1/2) (square lattice (pi,0)) wavevector, the wavevector of interest in other Fe-based superconductors, that extend to energies at least as high as 300 meV. Most importantly, the spin excitations in Fe1+yTe1-xSex exhibit four-fold symmetry about the (1,0) (square lattice (pi,pi)) wavevector and are described by the identical wavevector as the normal state spin excitations in the high-TC cuprates8-12 demonstrating a commonality between the magnetism in these classes of materials which perhaps extends to a common origin for superconductivity., Comment: 19 pages, 5 figures

We report neutron scattering measurements on single crystals of BaFe$_{1.92}$Co$_{0.08}$As$_2$. The magnetic Bragg peak intensity is reduced by 6 % upon cooling through T$_C$. The spin dynamics exhibit a gap of 8 meV with anisotropic three-dimensional (3d) interactions. Below T$_C$ additional intensity appears at an energy of $\sim$4.5(0.5) meV similar to previous observations of a spin resonance in other Fe-based superconductors. No further gapping of the spin excitations is observed below T$_C$ for energies down to 2 meV. These observations suggest the redistribution of spectral weight from the magnetic Bragg position to a spin resonance demonstrating the direct competition between static magnetic order and superconductivity., Comment: 4 pages, 4 figures

Inelastic neutron scattering measurements on single crystals of superconducting BaFe1.84Co0.16As2 reveal a magnetic excitation located at wavevectors (1/2 1/2 L) in tetragonal notation. On cooling below TC, a clear resonance peak is observed at this wavevector with an energy of 8.6(0.5) meV, corresponding to 4.5(0.3) kBTC. This is in good agreement with the canonical value of 5 kBTC observed in the cuprates. The spectrum shows strong dispersion in the tetragonal plane but very weak dispersion along the c-axis, indicating that the magnetic fluctuations are two-dimensional in nature. This is in sharp contrast to the anisotropic three dimensional spin excitations seen in the undoped parent compounds., Comment: Include additional data showing dispersion

By means of neutron scattering we show that the high-temperature precursor to the hidden order state of the heavy fermion superconductor URu$_{2}$Si$_{2}$ exhibits heavily damped incommensurate paramagnons whose strong energy dispersion is very similar to that of the long-lived longitudinal f-spin excitations that appear below T$_{0}$. Since the underlying local f-exchange is preserved we expect only the f-d interactions to change across the phase transition and to cause the paramagnetic damping. The damping exhibits single-ion behavior independent of wave vector and vanishes below the hidden order transition. We suggest that this arises from a transition from valence fluctuations to a hybridized f-d state below T$_{0}$. Here we present evidence that the itinerant excitations, like those in chromium, are due to Fermi surface nesting of hole and electron pockets so that the hidden order phase likely originates from a Fermi-surface instability. We identify wave vectors that span nested regions of a band calculation and that match the neutron spin crossover from incommensurate to commensurate on approach to the hidden order phase., Comment: 4 pages, 4 figures, to be submitted to PRL

We report muon spin relaxation ($\mu$SR) and magnetic susceptibility measurements on Cu(Cl,Br)La(Nb,Ta)$_{2}$O$_{7}$, which demonstrate: (a) the absence of static magnetism in (CuCl)LaNb$_{2}$O$_{7}$ down to 15 mK confirming a spin-gapped ground state; (b) phase separation between partial volumes with a spin-gap and static magnetism in (CuCl)La(Nb,Ta)$_{2}$O$_{7}$; (c) history-dependent magnetization in the (Nb,Ta) and (Cl,Br) substitution systems; (d) a uniform long-range collinear antiferromagnetic state in (CuBr)LaNb$_{2}$O$_{7}$; and (e) a decrease of N\'eel temperature with decreasing Br concentration $x$ in Cu(Cl$_{1-x}$Br$_{x}$)LaNb$_{2}$O$_{7}$ with no change in the ordered Cu moment size for $0.33 \leq x \leq 1$. Together with several other $\mu$SR studies of quantum phase transitions in geometrically-frustrated spin systems, the present results reveal that the evolution from a spin-gap to a magnetically ordered state is often associated with phase separation and/or a first order phase transition., Comment: 10 pages 10 color figures; revised from letter paper style to full paper style; Figs. 2, 4, 5, 7c, 10 newly added

Transverse-field muon spin rotation measurements of overdoped La2-xSrxCuO4 reveal a large broadening of the local magnetic field distribution in response to applied field, persisting to high temperatures. The field-response is approximately Curie-Weiss like in temperature and is largest for the highest doping investigated. Such behaviour is contrary to the canonical Fermi-liquid picture commonly associated with the overdoped cuprates and implies extensive heterogeneity in this region of the phase diagram. A possible explanation for the result lies in regions of staggered magnetization about dopant cations, analogous to what is argued to exist in underdoped systems., Comment: 4 pages, 4 figures; substantial changes; To be published in Physical Review B

Muon spin relaxation (MuSR) measurements in iron oxy-pnictide systems have revealed: (1) commensurate long-range order in undoped LaOFeAs; (2) Bessel function line shape in La(O0.97F0.03)FeAs which indicates possible incommensurate or stripe magnetism; (3) anomalous weak magnetism existing in superconducting LaOFeP, Ce(O0.84F0.16)FeAs, and Nd(O0.88F0.12)FeAs but absent in superconducting La(O0.92F0.08)FeAs; and (4) scaling of superfluid density and Tc in the Ce, La, and Nd-FeAs superconductors following a nearly linear relationship found in cuprates., Comment: 4 pages, 5 figures (color)

We have performed zero-field muon spin rotation measurements on single crystals of La_{2-x}Sr_{x}CuO_{4} to search for spontaneous currents in the pseudo-gap state. By comparing measurements on materials across the phase diagram, we put strict upper limits on any possible time-reversal symmetry breaking fields that could be associated with the pseudo-gap. Comparison between experimental limits and proposed circulating current states effectively eliminates the possibility that such states exist in this family of materials., Comment: Submitted to Phys. Rev. Lett. (2008)

One of the primary goals of modern condensed matter physics is to elucidate the nature of the ground state in various electronic systems. Many correlated electron materials, such as high temperature superconductors, geometrically frustrated oxides, and low-dimensional magnets are still the objects of fruitful study because of the unique properties which arise due to poorly understood many-body effects. Heavy fermion metals - materials which have high effective electron masses due to these effects - represent a class of materials with exotic properties, such as unusual magnetism, unconventional superconductivity, and "hidden order" parameters. The heavy fermion superconductor URu2Si2 has held the attention of physicists for the last two decades due to the presence of a "hidden order" phase below 17.5 K. Neutron scattering measurements indicate that the ordered moment is 0.03 $\mu_{B}$, much too small to account for the large heat capacity anomaly at 17.5 K. We present recent neutron scattering experiments which unveil a new piece of this puzzle - the spin excitation spectrum above 17.5 K exhibits well-correlated, itinerant-like spin excitations up to at least 10 meV emanating from incommensurate wavevectors. The gapping of these excitations corresponds to a large entropy release and explains the reduction in the electronic specific heat through the transition., Comment: 9 pages, 5 figures, high quality images available from Nature Replaced document with fixed figures

We have performed $\mu$SR studies on single crystals of SrCu$_2$(BO$_3$)$_2$, a quasi-two-dimensional spin system with a spin singlet ground state. We observe two different muon sites which we associate with muons located adjacent to the two inequivalent O sites. One site, presumed to be located in the Cu-O-Cu superexchange path, exhibits a large increase in the frequency shift with decreasing temperature which is unaffected by the singlet formation, indicating that the muon has locally broken the singlet bond. We have also performed $\mu$SR on single crystals of SrMg$_{0.05}$Cu$_{1.95}$(BO$_3$)$_2$, Sr$_{0.96}$La$_{0.04}$Cu$_2$(BO$_3$)$_2$, and Sr$_{0.95}$Na$_{0.05}$Cu$_2$(BO$_3$)$_2$. We have found that the frequency shifts of these doped samples are equivalent and contain three branches at low temperatures. Two of these branches map on to the branches observed in the pure sample reasonably well and so we attribute the third branch to effect of the dopants. Specifically, this third branch represents the case when the muon sits at a site in the superexchange path lacking a corresponding singlet, due to it already being broken as a result of doping. This then leads to the conclusion that singlets are broken in this system when it is doped both in and out of the CuBO$_3$ planes., Comment: 7 pages, 6 figures

Quantum phase transitions (QPTs) have been studied extensively in correlated electron systems. Characterization of magnetism at QPTs has, however, been limited by the volume-integrated feature of neutron and magnetization measurements and by pressure uncertainties in NMR studies using powderized specimens. Overcoming these limitations, we performed muon spin relaxation ($\mu$SR) measurements which have a unique sensitivity to volume fractions of magnetically ordered and paramagnetic regions, and studied QPTs from itinerant heli/ferro magnet to paramagnet in MnSi (single-crystal; varying pressure) and (Sr$_{1-x}$Ca$_{x}$)RuO$_{3}$ (ceramic specimens; varying $x$). Our results provide the first clear evidence that both cases are associated with spontaneous phase separation and suppression of dynamic critical behavior, revealed a slow but dynamic character of the ``partial order'' diffuse spin correlations in MnSi above the critical pressure, and, combined with other known results in heavy-fermion and cuprate systems, suggest a possibility that a majority of QPTs involve first-order transitions and/or phase separation., Comment: 11 pages, 4 figures, 21 authors, to appear in Nature Physics

muSR experiments on the geometrically frustrated spinel oxide, Li2Mn2O4, show the development of spin correlations over a range of length scales with decreasing temperature. Increased relaxation below 150 K is consistent with the onset of spin correlations. Below 50 K, spin order on a length scale, which is long range for the muSR probe, appears abruptly in temperature, consistent with prior neutron diffraction results. The oscillations in the zero field asymmetry are analyzed using a three frequency model. By locating the muon site this is shown to be consistent with the unexpected 2D q = root 3 x root 3 structure on the Kagome planes proposed originally from neutron data. Longitudinal field data demonstrate that some spin dynamics persist even at 2 K. Thus, a very complex magnetic ground state, featuring the co-existence of long length scale 2D ordering and significant spin dynamics, is proposed. This is unusual considering the 3D topology of the Mn3+ spins in this material., Comment: 9 pages, 9 figures, to be submitted to J. Phys. Cond. Matt

Muon spin relaxation ($\mu$SR) measurements in high transverse magnetic fields ($\parallel \hat c$) revealed strong field-induced quasi-static magnetism in the underdoped and Eu doped (La,Sr)$_{2}$CuO$_{4}$ and La$_{1.875}$Ba$_{0.125}$CuO$_{4}$, existing well above $T_{c}$ and $T_{N}$. The susceptibility-counterpart of Cu spin polarization, derived from the muon spin relaxation rate, exhibits a divergent behavior towards $T \sim 25$ K. No field-induced magnetism was detected in overdoped La$_{1.81}$Sr$_{0.19}$CuO$_{4}$, optimally doped Bi2212, and Zn-doped YBa$_{2}$Cu$_{3}$O$_{7}$., Comment: 4 pages, 4 color figures

Muon spin relaxation ($\mu$SR) measurements on the new layered cobalt oxide superconductor Na$_{0.35}$CoO$_{2}\cdot$1.3H$_{2}$O and its parent, non-superconducting compounds, have revealed unconventional nature of superconductivity through: (1) a small superfluid energy which implies a surprisingly high effective mass of the charge carriers, approximately 100 times the bare electron mass; (2) the superconducting transition temperature $T_{c}$ scaling with the superfluid energy following the correlations found in high-$T_{c}$ cuprate and some other two-dimensional superconductors; (3) an anisotropic pairing without broken time-reversal symmetry; and (4) the proximity of a magnetically ordered insulating phase at Na$_{0.5}$CoO$_{2}$ below $T_{N}$ = 53 K., Comment: 6 pages 4 figures: Contact Y.J. Uemura, E-mail: tomo@lorentz.phys.columbia.edu