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J. E. Greedan

Publications and source records attributed to J. E. Greedan.

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Magnetic and structural studies of G-phase compound Mn$_6$Ni$_{16}$Si$_7$

Transition metal compounds with complex crystal structures tend to demonstrate interesting magnetic coupling resulting in unusual magnetic properties. In this work, the structural and magnetic characterization of a single crystal of the Ni-Mn-Si based G-phase compound, Mn$_6$Ni$_{16}$Si$_7$, grown by the Czochralski method, is reported. In this structure isolated octahedral Mn$_6$ clusters form a f.c.c. lattice. As each octahedron consists of eight edge-sharing equilateral triangles, the possibility for geometric frustration exists. Magnetization and specific heat measurements showed two magnetic phase transitions at 197 K and 50 K, respectively. At 100 K neutron diffraction on powder samples shows a magnetic structure with k = (001) in which only four of the six Mn spins per cluster order along $<100>$ directions giving a two dimensional magnetic structure consistent with intra-cluster frustration. Below the 50 K phase transition the Mn spins cant away from $<100>$ directions and a weak moment develops on the two remaining Mn octahedral sites.

cond-mat.mtrl-sci↗

Spin gaps in the ordered states of La$_2$LiXO$_6$ (X = Ru, Os) and their relation to distortion of the cubic double perovskite structure in 4$d^3$ and 5$d^3$ magnets

Time-of-flight inelastic neutron scattering measurements have been carried out on polycrystalline samples of the 4$d^3$ and 5$d^3$ double pervoskite antiferromagnets La$_2$LiRuO$_6$ and La$_2$LiOsO$_6$. These reveal the development of an inelastic spin gap in La$_2$LiRuO$_6$ and La$_2$LiOsO$_6$ of $\sim$ 1.8(8) meV and 6(1) meV, below their respective ordering temperatures, $T_N$, $\sim$ 23.8 K and 30 K. The bandwidth of the spin excitations is shown to be $\sim$ 5.7(9) to 12(1) meV, respectively, at low temperatures. Spin gaps are surprising in such magnets as the t$_{2g}$ levels of Ru$^{5+}$ or Os$^{5+}$ are expected to be half-filled, resulting in an anticipated orbital singlet for both materials. We compare these results in monoclinic double perovskites La$_2$LiRuO$_6$ and La$_2$LiOsO$_6$ with those in cubic Ba$_2$YRuO$_6$ and Ba$_2$YOsO$_6$, as well as with those in the more strongly monoclinic La$_2$NaRuO$_6$, La$_2$NaOsO$_6$, and Sr$_2$ScOsO$_6$, and model the inelastic magnetic scattering with linear spin wave theory using minimal anisotropic exchange interactions. We discuss the possible role of the distortion of the face-centered cubic, double perovskite structure on the spin gap formation and geometric frustration in these materials, and show that $T_N$ scales with the top of the spin wave band in all members of these families that display long range order.

cond-mat.str-el↗

Neutron Diffraction and $μ$SR Studies of Two Polymorphs of Nickel Niobate (NiNb$_2$O$_6$)

Neutron diffraction and muon spin relaxation ($μ$SR) studies are presented for the newly characterized polymorph of NiNb$_2$O$_6$ ($β$-NiNb$_2$O$_6$) with space group P4$_2$/n and $μ$SR data only for the previously known columbite structure polymorph with space group Pbcn. The magnetic structure of the P4$_2$/n form was determined from neutron diffraction using both powder and single crystal data. Powder neutron diffraction determined an ordering wave vector $\vec{k}$ = ($\frac{1}{2},\frac{1}{2},\frac{1}{2}$). Single crystal data confirmed the same $\vec{k}$-vector and showed that the correct magnetic structure consists of antiferromagnetically-coupled chains running along the a or b-axes in adjacent Ni$^{2+}$ layers perpendicular to the c-axis, which is consistent with the expected exchange interaction hierarchy in this system. The refined magnetic structure is compared with the known magnetic structures of the closely related tri-rutile phases, NiSb$_2$O$_6$ and NiTa$_2$O$_6$. $μ$SR data finds a transition temperature of $T_N \sim$ 15 K for this system, while the columbite polymorph exhibits a lower $T_N =$ 5.7(3) K. Our $μ$SR measurements also allowed us to estimate the critical exponent of the order parameter $β$ for each polymorph. We found $β=$ 0.25(3) and 0.16(2) for the $β$ and columbite polymorphs respectively. The single crystal neutron scattering data gives a value for the critical exponent $β=$~0.28(3) for $β$-NiNb$_2$O$_6$, in agreement with the $μ$SR value. While both systems have $β$ values less than 0.3, which is indicative of reduced dimensionality, this effect appears to be much stronger for the columbite system. In other words, although both systems appear to well-described by $S = 1$ spin chains, the interchain interactions in the $β$-polymorph are likely much larger.

cond-mat.other↗

The frustrated FCC antiferromagnet Ba2YOsO6: structural characterization, magnetic properties and neutron scattering studies

We report the crystal structure, magnetization and neutron scattering measurements on the double perovskite Ba$_2$YOsO$_6$. The $Fm\overline{3}m$ space group is found both at 290~K and 3.5~K with cell constants $a_0 = 8.3541(4)$~Å and $8.3435(4)$~Å, respectively. Os$^{5+}$ ($5d^3$) ions occupy a non-distorted, geometrically frustrated face-centered-cubic (FCC) lattice. A Curie-Weiss temperature $θ= -772$~K suggests the presence of a large antiferromagnetic interaction and a high degree of magnetic frustration. A magnetic transition to long range antiferromagnetic order, consistent with a Type I FCC state below $T_{\rm N} \sim 69$~K, is revealed by magnetization, Fisher heat capacity and elastic neutron scattering, with an ordered moment of 1.65(6)~$μ_B$ on Os$^{5+}$. The ordered moment is much reduced from either the expected spin only value of $\sim 3 μ_B$ or the value appropriate to $4d^3$ Ru$^{5+}$ in isostructural Ba$_2$YRuO$_6$ of 2.2(1)~$μ_B$, suggesting a role for spin orbit coupling (SOC). Triple axis neutron scattering measurements of the order parameter suggest an additional first-order transition at $T = 67.45$~K, and the existence of a second ordered state. % Time-of-flight inelastic neutron results reveal a large spin gap $Δ\sim 17$~meV, unexpected for an orbitally quenched, $d^3$ electronic configuration. We discuss this in the context of the $\sim 5$~meV spin gap observed in the related Ru$^{5+}$, $4d^3$ cubic double perovskite Ba$_2$YRuO$_6$, and attribute the $\sim 3$ times larger gap to stronger SOC present in this heavier, $5d$, osmate system.

cond-mat.str-el↗

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 d.c. magnetic susceptibility, powder neutron diffraction and muon spin relaxation methods. The lattice parameter is a = 8.3619(6) A at 280K and cubic symmetry (Fm-3m) is retained to 3.5K with a = 8.3426(5) A. Curie-Weiss susceptibility behavior is observed for T > 100K and the derived constants are C = 0.3361(1)emu-K/mole and T_CW = -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/mole for a 5d^2 Os6+ configuration, indicating a major influence of spin-orbit coupling. Previous studies had detected both susceptibility and heat capacity anomalies near 50K 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 (muSR) data show clear long-lived oscillations indicative of long-range magnetic order below T_C = 50K. An estimate of the ordered moment on Os6+ is ~0.2 mu_B, based upon a comparison with muSR data for Ba2YRuO6 with a known ordered moment of 2.2 mu_B. These results are compared with those for isostructural Ba2YReO6 which contains Re5+, also 5d^2, and has a nearly identical unit cell constant, a = 8.3628(2) A. In contrast, Ba2YReO6 shows T_CW = -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. A comparison is made to recent theory on d^2 double perovskites.

cond-mat.str-el↗

Spin Gap and the Nature of the 4d3 Magnetic Ground State in the Frustrated FCC Antiferromagnet Ba2YRuO6

The geometrically frustrated double perovskite Ba2YRuO6 has magnetic 4d3 Ru5+ ions decorating an undistorted face-centered cubic (FCC) lattice. This material has been previously reported to exhibit commensurate long-range antiferromagnetic order below T_N = 36K, a factor f = 15 times lower than its Curie-Weiss temperature Theta_CW = -522 K, and purported short-range order to T* = 47K. We report new time-of-flight neutron spectroscopy of Ba2YRuO6 which shows the development of a 5 meV spin gap in the vicinity of the [100] magnetic ordering wavevector below T_N = 36K, with the transition to long-range order occurring at T* = 47K. We also report spin waves extending to 14 meV, a surprisingly small bandwidth in light of the large Theta_CW. We compare the spin gap and bandwidth to relevant neutron studies of the isostructural 4d1 material Ba2YMoO6,and discuss the results in the framework of relatively strong spin-orbit coupling expected in 4d magnetic systems.

cond-mat.str-el↗

Triplet and in-gap magnetic states in the ground state of the quantum frustrated FCC antiferromagnet Ba2YMoO6

The geometrically frustrated double perovskite Ba2YMoO6 is characterized by quantum s=1/2 spins at the Mo5+ sites of an undistorted face-centered cubic (FCC) lattice. Previous low-temperature characterization revealed an absence of static long-range magnetic order and suggested a non-magnetic spin-singlet ground state. We report new time-of-flight and triple-axis neutron spectroscopy of Ba2YMoO6 that shows a 28 meV spin excitation with a bandwidth of ~4 meV, which vanishes above ~125 K. We identify this as the singlet-triplet excitation out of a singlet ground state, and further identify a weaker continuum of magnetic states within the gap, reminiscent of spin-polaron states arising due to weak disorder.

cond-mat.str-el↗

Magnetic properties of the geometrically frustrated S=1/2 antiferromagnets, La2LiMoO6 and Ba2YMoO6, with the B-site ordered double perovskite structure: Evidence for a Collective Spin Singlet Ground State

Two B-site ordered double perovskites, La2LiMoO6 and Ba2YMoO6, based on the S = 1/2 ion, Mo5+, have been investigated in the context of geometric magnetic frustration. Powder neutron diffraction, heat capacity, susceptibility, muon spin relaxation(_SR), and 89Y NMR- including MAS NMR- data have been collected. La2LiMoO6 deviates strongly from simple Curie-Weiss paramagnetic behavior below 150K and zero-field cooled/ field cooled (ZFC/FC)irreversibility occurs below 20K with a weak, broad susceptibility maximum near 5K in the ZFC data. A Curie-Weiss fit shows a reduced mu_eff=1.42μ_B, (spin only = 1.73 muB) and a Weiss temperature, θ_c, which depends strongly on the temperature range of the fit. Powder neutron diffraction, heat capacity and 7Li NMR show no evidence for long range magnetic order to 2K. On the other hand oscillations develop below 20K in muSR indicating at least short range magnetic correlations. Susceptibility data for Ba2YMoO6 also deviate strongly from the C-W law below 150K with a similarly reduced mu_eff = 1.72μ_B and θ_c = - 219(1)K. Heat capacity, neutron powder diffraction and muSR data show no evidence for long range order to 2K but a very broad maximum appears in the heat capacity. The 89Y NMR paramagnetic Knight shift shows a remarkable local spin susceptibility behavior below about 70K with two components from roughly equal sample volumes, one indicating a singlet state and the other a strongly fluctuating paramagnetic state. Further evidence for a singlet state comes from the behavior of the relaxation rate, 1/T1. These results are discussed and compared with those from other isostructural S = 1/2 materials and those based on S = 3/2 and S = 1.

cond-mat.str-el↗

The Anderson-Mott transition induced by hole-doping in Nd1-xTiO3

The insulator/metal transition induced by hole-doping due to neodymium vacancies of the Mott- Hubbard antiferromagnetic insulator, Nd1-xTiO3, is studied over the composition range 0.010(6) < x < 0.243(10). Insulating p-types conduction is found for x < 0.071(10). Anderson localization in the presence of a Mott-Hubbard gap, is the dominant localization mechanism for the range of 0.074(10) < x < 0.089(1) samples. For x < 0.089(1), n-type conduction is observed and the activation energy extrapolates to zero by x < 0.1. The 0.095(8) < x < 0.203(10) samples are Fermi-liquid metals and the effects of strong electronic correlations are evident near the metal-to-insulator boundaries in features such as large Fermi liquid T2 coefficients. For 0.074(9) < x < 0.112(4), a weak negative magnetoresistance is found below ~ 15 K and it is attributed to the interaction of conduction electrons with Nd3+ magnetic moments. Combining information from our companion study of the magnetic properties of Nd1-xTiO3 solid solution, a phase diagram is proposed. The main conclusions are that long range antiferromagnetic order disappears before the onset of metallic behavior and that the Anderson-Mott transition occurs over a finite range of doping levels. Our results differ from conclusions drawn from a similar study on the hole doped Nd1-xCaxTiO3 system which found the co-existence of antiferromagnetic order and metallic behavior and that the Mott transition occurs at a discrete doping level.

cond-mat.str-el↗

2D Kagome Ordering in the 3D Frustrated Spinel Li2Mn2O4

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.

cond-mat.str-el↗

Magnetic Ordering in the Spin-Ice Candidate Ho$_2$Ru$_2$O$_7$

Neutron scattering measurements on the spin-ice candidate material Ho$_2$Ru$_2$O$_7$ have revealed two magnetic transitions at T $\sim$ 95 K and T $\sim$ 1.4 K to long-range ordered states involving the Ru and Ho sublattices, respectively. Between these transitions, the Ho$^{3+}$ moments form short-ranged ordered spin clusters. The internal field provided by the ordered S=1 Ru$^{4+}$ moments disrupts the fragile spin-ice state and drives the Ho$^{3+}$ moments to order. We have directly measured a slight shift in the Ho$^{3+}$ crystal field levels at 95 K from the Ru ordering.

cond-mat.stat-mech↗

Aging and memory properties of topologically frustrated magnets

The model 2d kagome system (H3O)Fe3(SO4)2(OH)6 and the 3d pyrochlore Y2Mo2O7 are two well characterized examples of low-disordered frustrated antiferromagnets which rather then condensing into spin liquid have been found to undergo a freezing transition with spin glass-like properties. We explore more deeply the comparison of their properties with those of spin glasses, by the study of characteristic rejuvenation and memory effects in the non-stationary susceptibility. While the pyrochlore shows clear evidence for these non-trivial effects, implying temperature selective aging, that is characteristic of a wide hierarchical distribution of equilibration processes, the kagome system does n not show clearly these effects. Rather, it seems to evolve towards the same final state independently of temperature.

cond-mat.dis-nn↗

Magnetic and Thermodynamic Properties of the Collective Paramagnet-Spin Liquid Pyrochlore Tb2Ti2O7

In a recent letter [Phys. Rev. Lett. {\bf 82}, 1012 (1999)] it was found that the Tb$^{3+}$ magnetic moments in the Tb$_2$Ti$_2$O$_7$ pyrochlore lattice of corner-sharing tetrahedra remain in a {\it collective paramagnetic} state down to 70mK. In this paper we present results from d.c. magnetic susceptibility, specific heat data, inelastic neutron scattering measurements, and crystal field calculations that strongly suggest that (1) the Tb$^{3+}$ ions in Tb$_2$Ti$_2$O$_7$ possess a moment of approximatively 5$μ_{\rm B}$, and (2) the ground state $g-$tensor is extremely anisotropic below a temperature of $O(10^0)$K, with Ising-like Tb$^{3+}$ magnetic moments confined to point along a local cubic $<111>$ diagonal (e.g. towards the middle of the tetrahedron). Such a very large easy-axis Ising like anisotropy along a $<111>$ direction dramatically reduces the frustration otherwise present in a Heisenberg pyrochlore antiferromagnet. The results presented herein underpin the conceptual difficulty in understanding the microscopic mechanism(s) responsible for Tb$_2$Ti$_2$O$_7$ failing to develop long-range order at a temperature of the order of the paramagnetic Curie-Weiss temperature $θ_{\rm CW} \approx -10^1$K. We suggest that dipolar interactions and extra perturbative exchange coupling(s)beyond nearest-neighbors may be responsible for the lack of ordering of Tb$_2$Ti$_2$O$_7$.

cond-mat.dis-nn↗

Transition to Long Range Magnetic Order in the Highly Frustrated Insulating Pyrochlore Antiferromagnet Gd_2Ti_2O_7

Experimental evidence from measurements of the a.c. and d.c. susceptibility, and heat capacity data show that the pyrochlore structure oxide, Gd_2Ti_2O_7, exhibits short range order that starts developing at 30K, as well as long range magnetic order at $T\sim 1$K. The Curie-Weiss temperature, $θ_{CW}$ = -9.6K, is largely due to exchange interactions. Deviations from the Curie-Weiss law occur below $\sim$10K while magnetic heat capacity contributions are found at temperatures above 20K. A sharp maximum in the heat capacity at $T_c=0.97$K signals a transition to a long range ordered state, with the magnetic specific accounting for only $\sim$ 50% of the magnetic entropy. The heat capacity above the phase transition can be modeled by assuming that a distribution of random fields acts on the $^8S_{7/2}$ ground state for Gd$^{3+}$. There is no frequency dependence to the a.c. susceptibility in either the short range or long range ordered regimes, hence suggesting the absence of any spin-glassy behavior. Mean field theoretical calculations show that no long range ordered ground state exists for the conditions of nearest-neighbor antiferromagnetic exchange and long range dipolar couplings. At the mean-field level, long range order at various commensurate or incommensurate wave vectors is found only upon inclusion of exchange interactions beyond nearest-neighbor exchange and dipolar coupling. The properties of Gd$_2Ti_2O_7 are compared with other geometrically frustrated antiferromagnets such as the Gd_3Ga_5O_{12} gadolinium gallium garnet, RE_2Ti_2O_7 pyrochlores where RE = Tb, Ho and Tm, and Heisenberg-type pyrochlore such as Y_2Mo_2O_7, Tb_2Mo_2O_7, and spinels such as ZnFe_2O_4

cond-mat.dis-nn↗

Weak pseudogap in crystals of Pb2Sr2(Y,Ca)Cu3O8+d

We report on NMR measurements in underdoped Pb2Sr2(Y,Ca)Cu3O8+d crystals. A pseudogap is observed in the Knight shift and spin-lattice relaxation rate. In contrast to other underdoped compounds, the pseudogap observed in the Knight shift is weak and occurs at a significantly lower temperature. On the other hand, the effect the pseudogap has on spin-lattice relaxation is quite similar to that in other compounds. The contrast between weak and strong pseudogaps is discussed.

cond-mat.supr-con↗

Muon Spin Relaxation Investigation of the Spin Dynamics of Geometrically Frustrated Antiferromagnets Y2Mo2O7 and Tb2Mo2O7 Static Critical Behavior of the Spin-Freezing

The spin dynamics of geometrically frustrated pyrochlore antiferromagnets Y2Mo2O7 and Tb2Mo2O7 have been investigated using muon spin relaxation. A dramatic slowing down of the moment fluctuations occurs as one approaches the spin freezing temperatures (TF=22 K and 25 K respectively) from above. Below TF there is a disordered magnetic state similar to that found in a spin glass but with a residual muon spin relaxation rate at low temperatures. These results show that there is a large density of states for magnetic excitations in these systems near zero energy.

cond-mat↗

Static Critical Behavior of the Spin-Freezing Transition in the Geometrically Frustrated Pyrochlore Antiferromagnet Y2Mo2O7

Some frustrated pyrochlore antiferromagnets, such as Y2Mo2O7, show a spin-freezing transition and magnetic irreversibilities below a temperature Tf similar to what is observed nonlinear magnetization measurements on Y2Mo2O7 that provide strong evidence that there is an underlying thermodynamic phase transition at Tf, which is characterized by critical exponents γ\approx 2.8 and β\approx 0.8. These values are typical of those found in random spin glasses, despite the fact that the level of random disorder in Y2Mo2O7 is immeasurably small.

cond-mat.dis-nn↗