Planar XY magnetic glass state in the Gd2ScNbO7pyrochlore.

Here a spin glass system with emergent planar ordered spin clusters is investigated. The mixed B-site pyrochlore Gd2ScNbO7has been synthesized and characterized through a variety of techniques, including x-ray diffraction, magnetic susceptibility, muon spin relaxation, heat capacity and neutron scattering. Despite a Curie-Weiss temperature of -3.93(3) K, indicating net antiferromagnetic interactions, no signs of long ranged magnetic ordering are found down toT= 0.3 K. Instead, a disordered magnetic state emerges with a small correlation length of 2.1(1) Å of single tetrahedra. A Reverse Monte Carlo analysis of the polarized neutron scattering data reveals short-range antiferromagnetic order with emergent XY spin ordering similar to the parent pyrochlore compounds. Muon spin relaxation, and AC susceptibility measurements confirm that the magnetization condenses into a glass, with 10 % of the potential entropy missing in the specific heat. This magnetic ground state is similar to what is observed in Gd2Sn2O7just above the ordering temperature, without the eventual long-range ordering at low temperature.

Quantum Critical Point in the Itinerant Ferromagnet Ni_{1-x}Rh_{x}.

We report a chemical substitution-induced ferromagnetic quantum critical point in polycrystalline Ni_{1-x}Rh_{x} alloys. Through magnetization and muon spin relaxation measurements, we show that the ferromagnetic ordering temperature is suppressed continuously to zero at x_{crit}=0.375 while the magnetic volume fraction remains 100% up to x_{crit}, pointing to a second order transition. Non-Fermi liquid behavior is observed close to x_{crit}, where the electronic specific heat C_{el}/T diverges logarithmically, while immediately above x_{crit} the volume thermal expansion coefficient α_{V}/T and the Grüneisen ratio Γ=α_{V}/C_{el} both diverge logarithmically in the low temperature limit, further indication of a ferromagnetic quantum critical point in Ni_{1-x}Rh_{x}.

Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce_{2}Zr_{2}O_{7}.

Neutron scattering measurements on the pyrochlore magnet Ce_{2}Zr_{2}O_{7} reveal an unusual crystal field splitting of its lowest J=5/2 multiplet, such that its ground-state doublet is composed of m_{J}=±3/2, giving these doublets a dipole-octupole (DO) character with local Ising anisotropy. Its magnetic susceptibility shows weak antiferromagnetic correlations with θ_{CW}=-0.4(2) K, leading to a naive expectation of an all-in, all-out ordered state at low temperatures. Instead, our low-energy inelastic neutron scattering measurements show a dynamic quantum spin ice state, with suppressed scattering near |Q|=0, and no long-range order at low temperatures. This is consistent with recent theory predicting symmetry-enriched U(1) quantum spin liquids for such DO doublets decorating the pyrochlore lattice. Finally, we show that disorder, especially oxidation of powder samples, is important in Ce_{2}Zr_{2}O_{7} and could play an important role in the low-temperature behavior of this material.

Low-carrier density and fragile magnetism in a Kondo lattice system.

Kondo-based semimetals and semiconductors are of extensive current interest as a viable platform for strongly correlated states in the dilute carrier limit. It is thus important to explore the routes to understand such systems. One established pathway is through the Kondo effect in metallic nonmagnetic analogs, in the so called half-filling case of one conduction electron and one 4f electron per site. Here, we demonstrate that Kondo-based semimetals develop out of conduction electrons with a low-carrier density in the presence of an even number of rare-earth sites. We do so by studying the Kondo material Yb3Ir4Ge13 along with its closed-4f -shell counterpart, Lu3Ir4Ge13. Through magnetotransport, optical conductivity, and thermodynamic measurements, we establish that the correlated semimetallic state of Yb3Ir4Ge13 below its Kondo temperature originates from the Kondo effect of a low-carrier conduction-electron background. In addition, it displays fragile magnetism at very low temperatures, which in turn, can be tuned to a Griffiths-phase-like regime through Lu-for-Yb substitution. These findings are connected with recent theoretical studies in simplified models. Our results can pave the way to exploring strong correlation physics in a semimetallic environment.

µSR study of spin freezing and persistent spin dynamics in NaCaNi2F7.

A new pyrochlore compound, NaCaNi2F7, was recently synthesized and has a single magnetic site with spin-1 Ni2+ . We present zero field and longitudinal field muon spin rotation (µSR) measurements on this pyrochlore. Density functional theory calculations show that the most likely muon site is located between two fluorine ions, but off-centre. A characteristic F-µ-F muon spin polarization function is observed at high temperatures where Ni spin fluctuations are sufficiently rapid. The Ni2+ spins undergo spin freezing into a disordered ground state below 4 K, with a characteristic internal field strength of 140 G. Persistent Ni spin dynamics are present to our lowest temperatures (75 mK), a feature characteristic of many geometrically frustrated magnetic systems.

Phase Competition in the Palmer-Chalker XY Pyrochlore Er_{2}Pt_{2}O_{7}.

We report neutron scattering measurements on Er_{2}Pt_{2}O_{7}, a new addition to the XY family of frustrated pyrochlore magnets. Symmetry analysis of our elastic scattering data shows that Er_{2}Pt_{2}O_{7} orders into the k=0, Γ_{7} magnetic structure (the Palmer-Chalker state), at T_{N}=0.38 K. This contrasts with its sister XY pyrochlore antiferromagnets Er_{2}Ti_{2}O_{7} and Er_{2}Ge_{2}O_{7}, both of which order into Γ_{5} magnetic structures at much higher temperatures, T_{N}=1.2 and 1.4 K, respectively. In this temperature range, the magnetic heat capacity of Er_{2}Pt_{2}O_{7} contains a broad anomaly centered at T^{*}=1.5 K. Our inelastic neutron scattering measurements reveal that this broad heat capacity anomaly sets the temperature scale for strong short-range spin fluctuations. Below T_{N}=0.38 K, Er_{2}Pt_{2}O_{7} displays a gapped spin-wave spectrum with an intense, flat band of excitations at lower energy and a weak, diffusive band of excitations at higher energy. The flat band is well described by classical spin-wave calculations, but these calculations also predict sharp dispersive branches at higher energy, a striking discrepancy with the experimental data. This, in concert with the strong suppression of T_{N}, is attributable to enhanced quantum fluctuations due to phase competition between the Γ_{7} and Γ_{5} states that border each other within a classically predicted phase diagram.

µSR investigation of a new diluted magnetic semiconductor Li(Zn,Mn,Cu)As with Mn and Cu codoping at the same Zn sites.

We report the successful synthesis and characterization of a new type I-II-V bulk form diluted magnetic semiconductor (DMS) Li(Zn,Mn,Cu)As, in which charge and spin doping are decoupled via (Cu,Zn) and (Mn,Zn) substitution at the same Zn sites. Ferromagnetic transition temperature up to ∼33 K has been observed with a coercive field ∼40 Oe for the 12.5% doping level. µSR measurements confirmed that the magnetic volume fraction reaches nearly 100% at 2 K, and the mechanism responsible for the ferromagnetic interaction in this system is the same as other bulk form DMSs.

Long-range magnetic order in the 5d(2) double perovskite Ba2CaOsO6: comparison with spin-disordered Ba2YReO6.

The B-site ordered double perovskite Ba2CaOsO6 was studied by dc magnetic susceptibility, powder neutron diffraction and muon spin relaxation methods. The lattice parameter is a = 8.3619(6) Å at 280 K and cubic symmetry [Formula: see text] is retained to 3.5 K with a = 8.3462(7) Å. Curie-Weiss susceptibility behaviour is observed for T > 100 K and the derived constants are C = 0.3361(3) emu K mol(-1) and ΘCW = -156.2(3) K, in excellent agreement with literature values. This Curie constant is much smaller than the spin-only value of 1.00 emu K mol(-1) for a 5d(2) Os(6+) configuration, indicating a major influence of spin-orbit coupling. Previous studies had detected both susceptibility and heat capacity anomalies near 50 K but no definitive conclusion was drawn concerning the nature of the ground state. While no ordered Os moment could be detected by powder neutron diffraction, muon spin relaxation (µSR) data show clear long-lived oscillations indicative of a continuous transition to long-range magnetic order below TC = 50 K. An estimate of the ordered moment on Os(6+) is ∼ 0.2 µB, based upon a comparison with µSR data for Ba2YRuO6 with a known ordered moment of 2.2 µB. These results are compared with those for isostructural Ba2YReO6 which contains Re(5+), also 5d(2), and has a nearly identical unit cell constant, a = 8.36278(2) Å-a structural doppelgänger. In contrast, Ba2YReO6 shows ΘCW = - 616 K, and a complex spin-disordered and, ultimately, spin-frozen ground state below 50 K, indicating a much higher level of geometric frustration than in Ba2CaOsO6. The results on these 5d(2) systems are compared to recent theory, which predicts a variety of ferromagnetic and antiferromagnetic ground states. In the case of Ba2CaOsO6, our data indicate that a complex four-sublattice magnetic structure is likely. This is in contrast to the spin-disordered ground state in Ba2YReO6, despite a lack of evidence for structural disorder, for which theory currently provides no clear explanation.

Incipient ferromagnetism in Tb2Ge2O7: application of chemical pressure to the enigmatic spin-liquid compound Tb2Ti2O7.

After nearly 20 years of study, the origin of the spin-liquid state in Tb2Ti2O7 remains a challenge for experimentalists and theorists alike. To improve our understanding of the exotic magnetism in Tb2Ti2O7, we synthesize a chemical pressure analog: Tb2Ge2O7. Substitution of titanium by germanium results in a lattice contraction and enhanced exchange interactions. We characterize the magnetic ground state of Tb2Ge2O7 with specific heat, ac and dc magnetic susceptibility, and polarized neutron scattering measurements. Akin to Tb2Ti2O7, there is no long-range order in Tb2Ge2O7 down to 20 mK. The Weiss temperature of -19.2(1) K, which is more negative than that of Tb2Ti2O7, supports the picture of stronger antiferromagnetic exchange. Polarized neutron scattering of Tb2Ge2O7 reveals that liquidlike correlations dominate in this system at 3.5 K. However, below 1 K, the liquidlike correlations give way to intense short-range ferromagnetic correlations with a length scale similar to the Tb-Tb nearest neighbor distance. Despite stronger antiferromagnetic exchange, the ground state of Tb2Ge2O7 has ferromagnetic character, in stark contrast to the pressure-induced antiferromagnetic order observed in Tb2Ti2O7.

New diluted ferromagnetic semiconductor with Curie temperature up to 180 K and isostructural to the '122' iron-based superconductors.

Diluted magnetic semiconductors have received much attention due to their potential applications for spintronics devices. A prototypical system (Ga,Mn)As has been widely studied since the 1990s. The simultaneous spin and charge doping via hetero-valent (Ga(3+),Mn(2+)) substitution, however, resulted in severely limited solubility without availability of bulk specimens. Here we report the synthesis of a new diluted magnetic semiconductor (Ba(1-x)K(x))(Zn(1-y)Mn(y))(2)As(2), which is isostructural to the 122 iron-based superconductors with the tetragonal ThCr(2)Si(2) (122) structure. Holes are doped via (Ba(2+), K(1+)) replacements, while spins via isovalent (Zn(2+),Mn(2+)) substitutions. Bulk samples with x=0.1-0.3 and y=0.05-0.15 exhibit ferromagnetic order with T(C) up to 180 K, which is comparable to the highest T(C) for (Ga,Mn)As and significantly enhanced from T(C) up to 50 K of the '111'-based Li(Zn,Mn)As. Moreover, ferromagnetic (Ba,K)(Zn,Mn)(2)As(2) shares the same 122 crystal structure with semiconducting BaZn(2)As(2), antiferromagnetic BaMn(2)As(2) and superconducting (Ba,K)Fe(2)As(2), which makes them promising for the development of multilayer functional devices.

Vibrating-coil magnetometry of the spin liquid properties of Tb2Ti2O7.

We have explored the spin liquid state in Tb(2)Ti(2)O(7) with vibrating-coil magnetometry down to ~0.04 K under magnetic fields up to 5 T. We observe magnetic history dependence below T*~0.2 K reminiscent of the classical spin ice systems Ho(2)Ti(2)O(7) and Dy(2)TiTi(2)O(7). The magnetic phase diagram inferred from the magnetization is essentially isotropic, without evidence of magnetization plateaus as anticipated for so-called quantum spin ice, predicted theoretically for [111] when quantum fluctuations renormalize the interactions. Instead, the magnetization for T≪T* agrees semiquantitatively with the predictions of "all-in-all-out" (AIAO) antiferromagnetism. Taken together, this suggests that the spin liquid state in Tb(2)Ti(2)O(7) is akin to an incipient AIAO antiferromagnet.

New magnetic phase diagram of (Sr,Ca)2RuO4.

High-T(c) cuprates, iron pnictides, organic BEDT and TMTSF, alkali-doped C(60), and heavy-fermion systems have superconducting states adjacent to competing states exhibiting static antiferromagnetic or spin density wave order. This feature has promoted pictures for their superconducting pairing mediated by spin fluctuations. Sr(2)RuO(4) is another unconventional superconductor which almost certainly has a p-wave pairing. The absence of known signatures of static magnetism in the Sr-rich side of the (Ca, Sr) substitution space, however, has led to a prevailing view that the superconducting state in Sr(2)RuO(4) emerges from a surrounding Fermi-liquid metallic state. Using muon spin relaxation and magnetic susceptibility measurements, we demonstrate here that (Sr,Ca)(2)RuO(4) has a ground state with static magnetic order over nearly the entire range of (Ca, Sr) substitution, with spin-glass behaviour in Sr(1.5)Ca(0.5)RuO(4) and Ca(1.5)Sr(0.5)RuO(4). The resulting new magnetic phase diagram establishes the proximity of superconductivity in Sr(2)RuO(4) to competing static magnetic order.

Spin ice: magnetic excitations without monopole signatures using muon spin rotation.

Theory predicts the low temperature magnetic excitations in spin ices consist of deconfined magnetic charges, or monopoles. A recent transverse-field (TF) muon spin rotation (µSR) experiment [S. T. Bramwell et al., Nature (London) 461, 956 (2009)] reports results claiming to be consistent with the temperature and magnetic field dependence anticipated for monopole nucleation-the so-called second Wien effect. We demonstrate via a new series of µSR experiments in Dy(2)Ti(2)O(7) that such an effect is not observable in a TF µSR experiment. Rather, as found in many highly frustrated magnetic materials, we observe spin fluctuations which become temperature independent at low temperatures, behavior which dominates over any possible signature of thermally nucleated monopole excitations.

Li(Zn,Mn)As as a new generation ferromagnet based on a I-II-V semiconductor.

In a prototypical ferromagnet (Ga,Mn)As based on a III-V semiconductor, substitution of divalent Mn atoms into trivalent Ga sites leads to severely limited chemical solubility and metastable specimens available only as thin films. The doping of hole carriers via (Ga,Mn) substitution also prohibits electron doping. To overcome these difficulties, Masek et al. theoretically proposed systems based on a I-II-V semiconductor LiZnAs, where isovalent (Zn,Mn) substitution is decoupled from carrier doping with excess/deficient Li concentrations. Here we show successful synthesis of Li(1+y)(Zn(1-x)Mn(x))As in bulk materials. Ferromagnetism with a critical temperature of up to 50 K is observed in nominally Li-excess (y=0.05-0.2) compounds with Mn concentrations of x=0.02-0.15, which have p-type metallic carriers. This is presumably due to excess Li in substitutional Zn sites. Semiconducting LiZnAs, ferromagnetic Li(Zn,Mn)As, antiferromagnetic LiMnAs, and superconducting LiFeAs systems share square lattice As layers, which may enable development of novel junction devices in the future.

Study of the ground state properties of LiHo(x)Y(1-x)F4 using muon spin relaxation.

LiHo(x)Y(1-x)F4 is an insulator where the magnetic Ho3+ ions have an Ising character and interact mainly through magnetic dipolar fields. We used the muon spin relaxation technique to study the nature of its ground state for samples with x ≤ 0.25. In contrast with some previous works, we did not find canonical spin glass behavior down to ≈ 15 mK. Instead, below ≈300 mK we observed temperature-independent dynamic magnetism characterized by a single correlation time. The 300 mK energy scale corresponds to the Ho3+ hyperfine interaction strength, suggesting that this interaction may be involved in the dynamic behavior of the system.

Interplay between structural, electronic, and magnetic degrees of freedom in Sr(3)Cr(2)O(8).

We present a theoretical investigation of the orbital ordering occurring in Sr(3)Cr(2)O(8) based on density functional theory calculations. We demonstrate that the strong electron correlation arising within the Cr-3d shell can clearly explain both the phase transition leading to the stabilization of its monoclinic C2/c space-group symmetry and its spin-singlet magnetic ground state. The relevance of the electronic structure determined theoretically is further established by comparison to high-resolution electron energy loss spectroscopy measurements.

Imaging the Fano lattice to 'hidden order' transition in URu(2)Si(2).

Within a Kondo lattice, the strong hybridization between electrons localized in real space (r-space) and those delocalized in momentum-space (k-space) generates exotic electronic states called 'heavy fermions'. In URu(2)Si(2) these effects begin at temperatures around 55 K but they are suddenly altered by an unidentified electronic phase transition at T(o) = 17.5 K. Whether this is conventional ordering of the k-space states, or a change in the hybridization of the r-space states at each U atom, is unknown. Here we use spectroscopic imaging scanning tunnelling microscopy (SI-STM) to image the evolution of URu(2)Si(2) electronic structure simultaneously in r-space and k-space. Above T(o), the 'Fano lattice' electronic structure predicted for Kondo screening of a magnetic lattice is revealed. Below T(o), a partial energy gap without any associated density-wave signatures emerges from this Fano lattice. Heavy-quasiparticle interference imaging within this gap reveals its cause as the rapid splitting below T(o) of a light k-space band into two new heavy fermion bands. Thus, the URu(2)Si(2) 'hidden order' state emerges directly from the Fano lattice electronic structure and exhibits characteristics, not of a conventional density wave, but of sudden alterations in both the hybridization at each U atom and the associated heavy fermion states.

Static magnetic order and superfluid density of RFeAs(O,F) (R=La,Nd,Ce) and LaFePO studied by muon spin relaxation: unusual similarities with the behavior of cuprate superconductors.

Muon spin relaxation measurements in iron-oxypnictide systems have revealed: (1) commensurate long-range order in undoped LaFeAsO; (2) a Bessel function line shape in LaFeAs(O0.97F0.03) which indicates possible incommensurate or stripe magnetism; (3) anomalous weak magnetism existing in superconducting LaFePO, CeFeAs(O0.084F0.16), and NdFeAs(O0.88F0.12) but absent in superconducting LaFeAs(O0.92F0.08); and (4) scaling of the superfluid density with T_{c} in the Ce-, La-, and Nd-FeAs superconductors following a nearly linear relationship found in cuprates.

Field-induced Bose-Einstein condensation of triplons up to 8 K in Sr3Cr2O8.

Single crystals of the spin dimer system Sr(3)Cr(2)O(8) have been grown for the first time. Magnetization, heat capacity, and magnetocaloric effect data up to 65 T reveal magnetic order between applied fields of H(c1) approximately 30.4 T and H(c2) approximately 62 T. This field-induced order persists up to T(c)(max) approximately 8 K at H approximately 44 T, the highest observed in any quantum magnet where H(c2) is experimentally accessible. We fit the temperature-field phase diagram boundary close to H(c1) using the expression T(c) = A(H-H(c1))(nu). The exponent nu = 0.65(2), obtained at temperatures much smaller than T(c)(max), is that of the 3D Bose-Einstein condensate (BEC) universality class. This finding strongly suggests that Sr(3)Cr(2)O(8) is a new realization of a triplon BEC where the universal regimes corresponding to both H(c1) and H(c2) are accessible at (4)He temperatures.

Itinerant spin excitations near the hidden order transition in URu(2)Si(2).

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). This suggests that there is a strongly hybridized character to the itinerant excitations observed previously above the hidden order transition. Here we present evidence that the itinerant excitations, like those in chromium, are due to Fermi surface nesting of hole and electron pockets; hence the hidden order phase probably originates from a Fermi surface instability. We identify wavevectors that span nested regions of a f-d hybridized band calculation and that match the neutron spin crossover from incommensurate to commensurate on approach to the hidden order phase.