No Arabic abstract
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.
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.
We report a comprehensive investigation of Ln2NiIrO6 (Ln = La, Pr, Nd) using thermodynamic and transport properties, neutron powder diffraction, resonant inelastic x-ray scattering, and density functional theory (DFT) calculations to investigate the role of A-site cations on the magnetic interactions in this family of hybrid 3d-5d-4f compositions. Magnetic structure determination using neutron diffraction reveals antiferromagnetism for La2NiIrO6, a collinear ferrimagnetic Ni/Ir state that is driven to long range antiferromagnetism upon the onset of Nd ordering in Nd2NiIrO6, and a non-collinear ferrimagnetic Ni/Ir sublattice interpenetrated by a ferromagnetic Pr lattice for Pr2NiIrO6. For Pr2NiIrO6 heat capacity results reveal the presence of two independent magnetic sublattices and transport resistivity indicates insulating behavior and a conduction pathway that is thermally mediated. First principles DFT calculation elucidates the existence of the two independent magnetic sublattices within Pr2NiIrO6 and offers insight into the behavior in La2NiIrO6 and Nd2NiIrO6. Resonant inelastic x-ray scattering is consistent with spin-orbit coupling splitting the t2g manifold of octahedral Ir4+ into a Jeff = 1/2 and Jeff = 3/2 state for all members of the series considered.
Comprehensive muon spin rotation/relaxation (muSR) and neutron powder diffraction (NPD) studies supported via bulk measurements have been performed on the ordered double perovskite Sr2YbRuO6 to investigate the nature of the magnetic ground state. Two sharp transitions at TN1 ~ 42 K and TN2 ~ 36 K have been observed in the static and dynamic magnetization measurements, coinciding with the heat capacity data. In order to confirm the origin of the observed phase transitions and the magnetic ground state, microscopic evidences are presented here. An initial indication of long-range magnetic ordering comes from a sharp drop in the muon initial asymmetry and a peak in the relaxation rate near TN1. NPD confirms that the magnetic ground state of Sr2YbRuO6 consists of an antiferromagnetic (AFM) structure with interpenetrating lattices of parallel Yb3+ and Ru5+ moments lying in the ab-plane and adopting a A-type AFM structure. Intriguingly, a small but remarkable change is observed in the long-range ordering parameters at TN2 confirming the presence of a weak spin reorientation (i.e. change in spin configuration) transition of Ru and Yb moments, as well as a change in the magnetic moment evolution of the Yb3+ spins at TN2. The temperature dependent behaviour of the Yb3+ and Ru5+ moments suggests that the 4d-electrons of Ru5+ play a dominating role in stabilizing the long range ordered magnetic ground state in the double perovskite Sr2YbRuO6 whereas only the Yb3+ moments show an arrest at TN2. The observed magnetic structure and the presence of a ferromagnetic interaction between Ru- and Yb- ions are explained with use of the Goodenough-Kanamori-Anderson (GKA) rules. Possible reasons for the presence of the second magnetic phase transition and of a compensation point in the magnetization data are linked to competing mechanisms of magnetic anisotropy.
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.
The magnetic structures and the magnetic phase transitions in the Mn-doped orthoferrite TbFeO$_3$ studied using neutron powder diffraction are reported. Magnetic phase transitions are identified at $T^mathrm{Fe/Mn}_N approx$ 295~K where a paramagnetic-to-antiferromagnetic transition occurs in the Fe/Mn sublattice, $T^mathrm{Fe/Mn}_{SR} approx$ 26~K where a spin-reorientation transition occurs in the Fe/Mn sublattice and $T^mathrm{R}_N approx$ 2~K where Tb-ordering starts to manifest. At 295~K, the magnetic structure of the Fe/Mn sublattice in TbFe$_{0.5}$Mn$_{0.5}$O$_3$ belongs to the irreducible representation $Gamma_4$ ($G_xA_yF_z$ or $Pbnm$). A mixed-domain structure of ($Gamma_1 + Gamma_4$) is found at 250~K which remains stable down to the spin re-orientation transition at $T^mathrm{Fe/Mn}_{SR}approx$ 26~K. Below 26~K and above 250~K, the majority phase ($> 80%$) is that of $Gamma_4$. Below 10~K the high-temperature phase $Gamma_4$ remains stable till 2~K. At 2~K, Tb develops a magnetic moment value of 0.6(2)~$mu_mathrm{B}/$f.u. and orders long-range in $F_z$ compatible with the $Gamma_4$ representation. Our study confirms the magnetic phase transitions reported already in a single crystal of TbFe$_{0.5}$Mn$_{0.5}$O$_3$ and, in addition, reveals the presence of mixed magnetic domains. The ratio of these magnetic domains as a function of temperature is estimated from Rietveld refinement of neutron diffraction data. Indications of short-range magnetic correlations are present in the low-$Q$ region of the neutron diffraction patterns at $T < T^mathrm{Fe/Mn}_{SR}$. These results should motivate further experimental work devoted to measure electric polarization and magnetocapacitance of TbFe$_{0.5}$Mn$_{0.5}$O$_3$.