No Arabic abstract
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=1.42mu_B, (spin only = 1.73 muB) and a Weiss temperature, theta_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 = 1.72mu_B and theta_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.
The recent discovery of Spin-ice is a spectacular example of non-coplanar spin arrangements that can arise in the pyrochlore A2B2O7 structure. We present magnetic and thermodynamic studies on the metallic-ferromagnet pyrochlore Sm2Mo2O7. Our studies, carried out on oriented crystals, suggest that the Sm spins have an ordered spin-ice ground state below about T* = 15 K. The temperature- and field-evolution of the ordered spin-ice state are governed by an antiferromagnetic coupling between the Sm and Mo spins. We propose that as a consequence of a robust feature of this coupling, the tetrahedra aligned with the external field adopt a 1-in, 3-out spin structure as opposed to 3-in, 1-out in dipolar spin ices, as the field exceeds a critical value.
Magnetic structures and the relationship between spin and charge-orbital orderings of an A-site ordered double-perovskite manganite SmBaMn2O6, an anticipated multiferroic material, were investigated by means of neutron diffraction. The spin arrangement in MnO2 planes perpendicular to the c axis is revealed to be the same as that in the A-site disordered half-doped manganites CE-type but the stacking pattern is found to be different displaying a unique twofold period. The temperature dependence of the superlattice magnetic and nuclear reflections clarifies that the antiferromagnetic spin ordering occurs at a temperature slightly lower than the temperature at which a rearrangement of the charge-orbital orderings occurs. The result evidences that the rearrangement leads the spin ordering. The intensities of the magnetic reflections are found to change across Tf = 10 K, suggesting a spin-flop by 90 [deg.] while keeping the Mn spin ordering pattern unchanged.
We present a model compound with a spin-1/2 frustrated square lattice, in which three ferromagnetic (F) interactions and one antiferromagnetic (AF) compet. Considering the effective spin-1 formed by the dominant F dimer, this square lattice can be mapped to a spin-1 spatially anisotropic triangular lattice. The magnetization curve exhibits gapped behavior indicative of a dominant one-dimensional (1D) AF correlation. In the field-induced gapless phase, the specific heat and magnetic susceptibility show a phase transition to an ordered state with 2D characteristics. These results indicate that the spin-1 Haldane state is extended to the 2D system. We demonstrate that the gapped ground state observed in the present spin-1/2 frustrated square lattice originates from the one-dimensionalization caused by frustration.
Exactly solvable frustrated quantum spin models consisting of a diamond unit structure are presented. The ground states are characterized by tetramer-dimer states with a macroscopic degeneracy in a certain range of isotropic exchange interaction. The lower bound of the excitation gap is exactly calculated to be finite and the bulk entropy in the limit of zero temperature remains finite depending on the shape of the boundary of system. Residual entropy is in a range of 0~6.1% of the entropy at high temperature for hexagonal diamond lattice and 0~8.4% for square diamond lattice. These diamond lattices are generalized to any dimensions and it is likely to be synthesized experimentally.
The magnetic ground state of double perovskite Sr2DyRuO6 has been investigated using muon spin rotation and relaxation (muSR), neutron powder diffraction (NPD) and inelastic neutron scattering (INS), in addition to heat capacity and magnetic susceptibility (ac and dc) measurements. A clear signature of a long-range ordered magnetic ground state has been observed in the heat capacity data, which exhibit two sharp anomalies at 39.5 and 36 K found as well in the magnetic data. Further confirmation of long-range magnetic ordering comes from a sharp drop in the muon initial asymmetry and a peak in the relaxation rate at 40 K, along with a weak anomaly near 36 K. Based on temperature dependent NPD, the low temperature magnetic structure contains two interpenetrating lattices of Dy and Ru5, forming an antiferromagnetic ground state below 39.5 K with magnetic propagation vector k = (0,0,0). The magnetic moments of Dy and Ru at 3.5 K are pointing along the crystallographic b-axis with values of muDy = 4.92(10) muB and muRu = 1.94(7) muB, respectively. The temperature dependence of the Ru moments follows a mean field type behaviour, while that of the Dy moments exhibits a deviation indicating that the primary magnetic ordering is induced by the order of the 4d electrons of Ru rather than that of its proper 4f Dy electrons. The origin of the second anomaly observed in the heat capacity data at 36.5 K must be connected to a very small spin reorientation as the NPD studies do not reveal any clear change in the observed magnetic Bragg peaks positions or intensities between these two transitions. INS measurements reveal the presence of crystal field excitations (CEF) in the paramagnetic state with overall CEF splitting of 73.8 meV, in agreement with the point change model calculations.