Non-magnetic ion site disorder effects on the quantum magnetism of a spin-1/2 equilateral triangular lattice antiferromagnet.

With the motivation to study how non-magnetic ion site disorder affects the quantum magnetism of Ba3CoSb2O9, a spin-1/2 equilateral triangular lattice antiferromagnet, we performed DC and AC susceptibility, specific heat, elastic and inelastic neutron scattering measurements on single crystalline samples of Ba2.87Sr0.13CoSb2O9with Sr doping on non-magnetic Ba2+ion sites. The results show that Ba2.87Sr0.13CoSb2O9exhibits (i) a two-step magnetic transition at 2.7 K and 3.3 K, respectively; (ii) a possible canted 120 degree spin structure at zero field with reduced ordered moment as 1.24µB/Co; (iii) a series of spin state transitions for bothH∥ab-plane andH∥c-axis. ForH∥ab-plane, the magnetization plateau feature related to the up-up-down phase is significantly suppressed; (iv) an inelastic neutron scattering spectrum with only one gapped mode at zero field, which splits to one gapless and one gapped mode at 9 T. All these features are distinctly different from those observed for the parent compound Ba3CoSb2O9, which demonstrates that the non-magnetic ion site disorder (the Sr doping) plays a complex role on the magnetic properties beyond the conventionally expected randomization of the exchange interactions. We propose the additional effects including the enhancement of quantum spin fluctuations and introduction of a possible spatial anisotropy through the local structural distortions.

Magnetic ordering in the Ising antiferromagnetic pyrochlore Nd2ScNbO7.

The question of structural disorder and its effects on magnetism is relevant to a number of spin liquid candidate materials. Although commonly thought of as a route to spin glass behaviour, here we describe a system in which the structural disorder results in long-range antiferromagnetic order due to local symmetry breaking. Nd2ScNbO7is shown to have a dispersionless gapped excitation observed in other neodymium pyrochlores belowTN= 0.37 K through polarized and inelastic neutron scattering. However the dispersing spin waves are not observed. This excited mode is shown to occur in only 14(2)% of the neodymium ions through spectroscopy and is consistent with total scattering measurements as well as the magnitude of the dynamic moment 0.26(2)µB. The remaining magnetic species order completely into the all-in all-out Ising antiferromagnetic structure. This can be seen as a result of local symmetry breaking due disordered Sc+3and Nb+5ions about theA-site. From this work, it has been established thatB-site disorder restores the dipole-like behaviour of the Nd+3ions compared to the Nd2B2O7parent series.

Dynamical ground state in the XY pyrochlore Yb2GaSbO7.

The magnetic ground state of the pyrochlore Yb2GaSbO7 has remained an enigma for nearly a decade. The persistent spin fluctuations observed by muon spin relaxation measurements at low temperatures have not been adequately explained for this material using existing theories for quantum magnetism. Here we report on the synthesis and characterisation of Yb2GaSbO7 to elucidate the central physics at play. Through DC and AC magnetic susceptibility, heat capacity, and neutron scattering experiments, we observe evidence for a dynamical ground state that makes Yb2GaSbO7 a promising candidate for disorder-induced spin-liquid or spin-singlet behaviour. This state is quite fragile, being tuned to a splayed ferromagnet in a modest magnetic field µ0Hc∼1.5T.

Evidence for negative thermal expansion in the superconducting precursor phase SmFeAsO.

The fluorine-doped rare-earth iron oxypnictide series SmFeAsO1-x F x (0 [Formula: see text] 0.10) was investigated with high resolution powder x-ray scattering. In agreement with previous studies (Margadonna et al 2009 Phys. Rev. B. 79 014503), the parent compound SmFeAsO exhibits a tetragonal-to-orthorhombic structural distortion at [Formula: see text] = 130 K which is rapidly suppressed by [Formula: see text] 0.10 deep within the superconducting dome. The change in unit cell symmetry is followed by a previously unreported magnetoelastic distortion at 120 K. The temperature dependence of the thermal expansion coefficient [Formula: see text] reveals a rich phase diagram for SmFeAsO: (i) a global minimum at 125 K corresponds to the opening of a spin-density wave instability as measured by pump-probe femtosecond spectroscopy (Mertelj et al 2010 Phys. Rev. B 81 224504) whilst (ii) a global maximum at 110 K corresponds to magnetic ordering of the Sm and Fe sublattices as measured by magnetic x-ray scattering (Nandi et al 2011 Phys. Rev. B 84 055419). At much lower temperatures than [Formula: see text], SmFeAsO exhibits a significant negative thermal expansion on the order of -40 ppm · K-1 in contrast to the behaviour of other rare-earth oxypnictides such as PrFeAsO (Kimber et al 2008 Phys. Rev. B 78 140503) and the actinide oxypnictide NpFeAsO (Klimczuk et al 2012 Phys. Rev. B 85 174506) where the onset of [Formula: see text] 0 only appears in the vicinity of magnetic ordering. Correlating this feature with the temperature and doping dependence of the resistivity and the unit cell parameters, we interpret the negative thermal expansion as being indicative of the possible condensation of itinerant electrons accompanying the opening of a SDW gap, consistent with transport measurements (Tropeano et al 2009 Supercond. Sci. Technol. 22 034004).

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.

Evidence for the confinement of magnetic monopoles in quantum spin ice.

Magnetic monopoles are hypothesised elementary particles connected by Dirac strings that behave like infinitely thin solenoids (Dirac 1931 Proc. R. Soc. A 133 60). Despite decades of searching, free magnetic monopoles and their Dirac strings have eluded experimental detection, although there is substantial evidence for deconfined magnetic monopole quasiparticles in spin ice materials (Castelnovo et al 2008 Nature 326 411). Here we report the detection of a hierarchy of unequally-spaced magnetic excitations via high resolution inelastic neutron spectroscopic measurements on the quantum spin ice candidate [Formula: see text] [Formula: see text] [Formula: see text]. These excitations are well-described by a simple model of monopole pairs bound by a linear potential (Coldea et al Science 327 177) with an effective tension of 0.642(8) K [Formula: see text] at 1.65 K. The success of the linear potential model suggests that these low energy magnetic excitations are direct spectroscopic evidence for the confinement of magnetic monopole quasiparticles in the quantum spin ice candidate [Formula: see text] [Formula: see text] [Formula: see text].

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.

Phase diagram and magnetic structures of the Co-bearing dugganites Pb3TeCo3A2O14 (A = V, P).

Exhibiting rich magnetic behaviour and potentially multiferroic properties, the dugganites, a Te(6+) containing subgroup of the langasite series, are an attractive family of compounds for future study. It was recently shown that Pb-bearing members of the dugganite series undergo distortions away from the P321 symmetry that is characteristic of the langasites. Here, we detail the consequences these distortions have on the magnetism exhibited by Pb3TeCo3V2O14 and Pb3TeCo3P2O14, solving the magnetic structures of both compounds with respect to a new supercell. Using neutron scattering and magnetic susceptibility measurements, we show that small applied magnetic fields can seriously perturb the delicate magnetic states in both of these systems. This is further demonstrated by presenting how doping P(5+) onto the nonmagnetic V(5+) site completely changes the magnetic structure from either of the end series members. Finally, it is shown using inelastic neutron scattering and magnetic susceptibility measurements that Pb3TeCo3V2O14 can be characterized using a model for isosceles trimers, which do not exist in the previously reported P321 subcell.

Chemical pressure effects on pyrochlore spin ice.

A comparison among the two sets of studied pyrochlore spin ices, Ho2Sn2O7, Ho2Ti2O7, and Ho2Ge2O7 with Ho3+ spins and Dy2Sn2O7, Dy2Ti2O7, and Dy2Ge2O7 with Dy3+ spins, shows that the application of chemical pressure through each set drives the system toward the antiferromagnetic phase boundary from the spin ice region, which agrees with the prediction of the "dipolar spin ice" model of den Hertog and Gingras. Among all the studied pyrochlore spin ices, Dy2Ge2O7 has the smallest ratio of Jnn/Dnn=-0.73.

Spin dynamics of the S = 5/2 2D triangular antiferromagnet Ba3NbFe3Si2O14.

We report pulse-field magnetization, ac susceptibility, and 100 GHz electron spin resonance (ESR) measurements on the S = 5/2 two-dimensional triangular compound Ba3NbFe3Si2O14 with the Néel temperature T(N) = 26 K. The magnetization curve shows an almost linear increase up to 60 T with no indication of a one-third magnetization plateau. An unusually large frequency dependence of the ac susceptibility in the temperature range of T = 20-100 K reveals a spin-glass behavior or superparamagnetism, signaling the presence of frustration-related slow magnetic fluctuations. The temperature dependence of the ESR linewidth exhibits two distinct critical regimes; (i) ΔH(pp)(T) is proportional to (T-T(N))(-p) with the exponent p = 0.2(1)-0.2(3) for temperatures above 27 K, and (ii) ΔH(pp)(T) is proportional to (T-T*)(-p) with T* = 12 K and p = 0.8(1)-0.8(4) for temperatures between 12 and 27 K. This is interpreted as indicating a dimensional crossover of magnetic interactions and the persistence of short-range correlations with a helically ordered state.

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.

Successive phase transitions and extended spin-excitation continuum in the S=1/2 triangular-lattice antiferromagnet Ba3CoSb2O9.

Using magnetic, thermal, and neutron measurements on single-crystal samples, we show that Ba3CoSb2O9 is a spin-1/2 triangular-lattice antiferromagnet with the c axis as the magnetic easy axis and two magnetic phase transitions bracketing an intermediate up-up-down phase in magnetic field applied along the c axis. A pronounced extensive neutron-scattering continuum above spin-wave excitations, observed below T(N), implies that the system is in close proximity to one of two spin-liquid states that have been predicted for a 2D triangular lattice.

High pressure route to generate magnetic monopole dimers in spin ice.

The gas of magnetic monopoles in spin ice is governed by one key parameter: the monopole chemical potential. A significant variation of this parameter could access hitherto undiscovered magnetic phenomena arising from monopole correlations, as observed in the analogous electrical Coulomb gas, like monopole dimerization, critical phase separation, or charge ordering. However, all known spin ices have values of chemical potential imposed by their structure and chemistry that place them deeply within the weakly correlated regime, where none of these interesting phenomena occur. Here we use high-pressure synthesis to create a new monopole host, Dy(2)Ge(2)O(7), with a radically altered chemical potential that stabilizes a large fraction of monopole dimers. The system is found to be ideally described by the classic Debye-Huckel-Bjerrum theory of charge correlations. We thus show how to tune the monopole chemical potential in spin ice and how to access the diverse collective properties of magnetic monopoles.

Absence of long-range magnetic ordering in the pyrochlore compound Er2Sn2O7.

The low temperature behaviour of powder Er2Sn2O7 samples has been studied by magnetic susceptibility, heat capacity, and neutron scattering experiments. We report here the absence of magnetic ordering down to 100 mK. Anomalies in the heat capacity can be accounted for through an analysis of the crystal field spectrum observed by inelastic neutron scattering spectroscopy. These new measurements on Er2Sn2O7 suggest a new lower bound for the frustration index of f = |Θ(CW)|/T(N) = 14/0.1 = 140, placing this compound into a highly frustrated regime.

Spin liquid state in the S = 1/2 triangular lattice Ba3CuSb2O9.

The synthesis and characterization of Ba3CuSb2O9, which has a layered array of Cu2+ spins in a triangular lattice, are reported. The magnetic susceptibility and neutron scattering experiments of this material show no magnetic ordering down to 0.2 K with a θ(CW) = -55 K. The magnetic specific heat reveals a T-linear dependence with a γ = 43.4 mJ K(-2) mol(-1) below 1.4 K. These observations suggest that Ba3CuSb2O9 is a new quantum spin liquid candidate with a S = 1/2 triangular lattice.

Short range ordering in the modified honeycomb lattice compound SrHo(2)O(4).

The low temperature behaviour of single crystalline SrHo(2)O(4) has been characterized by dc magnetic susceptibility, heat capacity, and neutron scattering experiments. Our results show that despite the lack of magnetic long-ranged ordering in the presence of strong antiferromagnetic correlations, SrHo(2)O(4) does not order down to 1.8 K. Elastic neutron scattering experiments show prominent magnetic diffuse scattering correlated with a broad feature in the dc susceptibility at T = 4 K, indicative of magnetic short-ranged ordering of the Ho(3) spins. Inelastic neutron scattering shows the presence of five crystal field levels up to 80 K in energy, in agreement with the integration of the magnetic specific heat component yielding Rln5 entropy release. The magnetic short-ranged ordering is fitted to a nearest neighbour interaction model with good agreement.

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.

Chemical pressure induced spin freezing phase transition in kagome pr langasites.

The 2D kagome system Pr3Ga5SiO14 has been previously identified as a spin-liquid candidate in zero field, displaying no magnetic long-ranged order down to at least 35 mK. Perturbations upon such systems, either under applied fields or applied pressure, should induce a spin freezing phase transition, but there are very few experimental realizations of this phenomena other than the well-studied 3D pyrochlore Tb2Ti2O7. In this Letter, we report the observation of a spin freezing phase transition in Pr3Ga5SiO14 through the application of chemical pressure--that is, through a systematic substitution on the Si site with larger ions and an elongation of the nearest-neighbor Pr-Pr distance in the kagome lattice. This results in a suppression of the T2 component of the heat capacity, and the reduction of the exchange constant eventually leads to dipolar-driven spin freezing.

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.

Absence of spin liquid behavior in Nd3Ga5SiO14 using magneto-optical spectroscopy.

We measured the low-lying crystal field levels of Nd3+ in Nd3Ga5SiO14 via magneto-optical spectroscopy and employed the extracted energies, magnetic moments, and symmetries to analyze the magnetic properties and test the spin liquid candidacy of this material. The exchange interaction is surprisingly small, a discovery that places severe constraints on models used to describe the ground state of this system. Further, it demonstrates the value of local-probe photophysical techniques for rare-earth-containing materials where bulk property measurements can be skewed by low-lying electronic structure.