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Register a new userMuon spin relaxation investigation of magnetic ordering in the hybrid organic-inorganic perovskites [(CH3)2NH2]M(HCOO)3, M = Ni,Co,Mn,Cu
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Muon spin relaxation measurements are reported on samples of dimethylammonium metal formates containing magnetic divalent nickel, cobalt, manganese, and copper ions. These hybrid organic-inorganic perovskites exhibit weak ferromagnetism and are, apart from the copper system, multiferroics with well separated magnetic and antiferroelectric transitions. We use muons to follow the sublattice magnetization, observing the effect of the spin reorientation transitions below TN and the criticality approaching TN. The multiferroic samples have three-dimensional antiferromagnetic interactions, but the copper sample shows quasi-one-dimensional behavior due to its Jahn-Teller distorted structure, with a ratio of its inter- and intrachain exchange constants j/J=0.037.
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In this work we explore the overall structural behaviour of the [(CH3)2NH2][Mn(HCOO)3] multiferroic compound across the temperature range where its ferroelectric transition takes place by means of calorimetry, thermal expansion measurements and variable temperature powder and single crystal X-ray diffraction. The results clearly proof the presence of structural phase transition at Tt ~187 K (temperature at which the dielectric transition occurs) that involves a symmetry change from R-3c to Cc, twinning of the crystals, a discontinuous variation of the unit cell parameters and unit cell volume, and a sharp first-order-like anomaly in the thermal expansion. In addition, the calorimetric results show a 3-fold order-disorder transition. The calculated pressure dependence of the transition temperature is rather large (dTt/dP = 4.6 $pm$ 0.1 K/kbar), so that it should be feasible to shift it to room temperature using adequate thermodynamic conditions, for instance by application of external pressure.
New double perovskites LaPbMSbO6, where M2+ = Mn2+, Co2+, and Ni2+, were synthesized as polycrystals by an aqueous synthetic route at temperatures below 1000 oC. All samples are monoclinic, space group P21/n, as obtained from Rietveld analysis of X-ray powder diffraction patterns. The distribution of M2+ and Sb5+ among the two octahedral sites have 3% of disorder for M2+ = Ni2+, whereas for M2+ = Mn2+ and Co2+ less disorder is found. The three samples have an antiferromagnetic transition, due to the antiferromagnetic coupling between M2+ through super-superexchange paths M2+ - O2- - Sb5+ - O2- - M2+. Transition temperatures are low: 8, 10 and 17 K for Mn2+, Co2+, and Ni2+ respectively, as a consequence of the relatively long distances between the magnetic ions M2+. Besides, for LaPbMnSbO6 a small transition at 45 K was found, with ferrimagnetic characteristics, possibly as a consequence of a small disorder between Mn2+ and Sb5+. This disorder would give additional and shorter interaction paths: superexchange Mn2+ - O2- - Mn2+.
We performed susceptibility, magnetization, specific heat, and single crystal neutron diffraction measurements on single crystalline BaMn$_2$Si$_2$O$_7$. Based on the results, we revisited its spin structure with a more accurate solution and constructed a magnetic phase diagram with applied field along the $b$-axis, which contains a spin flop transition around 6 T. We also used susceptibility, magnetization, and specific heat results confirmed the ferrimagnetic-like magnetism in polycrystalline BaCo$_2$Si$_2$O$_7$. Furthermore, we performed LSDA + U calculations for the BaM$_2$Si$_2$O$_7$ (M = Cu, Co, and Mn) system. Our discussions based on the comparison among the obtained magnetic exchange interactions suggest the different structures and electronic configurations are the reasons for the different magnetic properties among the system members.
Magnetic properties of silver(II) compounds have been of interest in recent years. In covalent compounds, the main mechanism of interaction between paramagnetic sites is the superexchange via the connecting ligand. To date, little is known of magnetic interactions between Ag(II) cations and other paramagnetic centres. It is because only a few compounds bearing Ag(II) cation and other paramagnetic transition metal cation are known experimentally. Recently the high-pressure synthesis of ternary silver(II) fluorides with 3d metal cations AgMF4 (M = Co, Ni, Cu) was predicted to be feasible. Here, we investigate the magnetic properties of these compounds in their diverse polymorphic forms. Using well established computational methods we predict superexchange pathways in AgMF4, evaluate coupling constants and calculate the impact of Ag(II) presence on superexchange between the other cations. The results indicate that the low-pressure form of AgCuF4, the only composed of stacked layers as the parent AgF2, would hold mainly Ag-Ag and Cu-Cu superexchange interactions. Upon compression, or with the nickel(II) cation, the Ag-M interactions in AgMF4 intensify, which is emphasized by an increase of Ag-M superexchange coupling constants and Ag-F-M angles. All the strongest Ag-M superexchange pathways are quasi-linear, leading to the formation of antiferromagnetic chains along the crystallographic directions. The impact of Ag(II) on M-M superexchange turns out to be moderate, due to factors connected to the crystal structure.
We report the synthesis, crystal structure and characterization by means of single crystal x-ray diffraction, neutron powder diffraction, magnetic, thermal and transport measurements of the new heavy fermion compounds Ce$_{2}$MAl$_{7}$Ge$_{4}$ (M = Co, Ir, Ni, Pd). These compounds crystallize in a noncentrosymmetic tetragonal space group P={4}2$_{1}$m, consisting of layers of square nets of Ce atoms separated by Ge-Al and M-Al-Ge blocks. Ce$_{2}$CoAl$_{7}$Ge$_{4}$, Ce$_{2}$IrAl$_{7}$Ge$_{4}$ and Ce$_{2}$NiAl$_{7}$Ge$_{4}$ order magnetically behavior below $T_{M}=$ 1.8, 1.6, and 0.8 K, respectively. There is no evidence of magnetic ordering in Ce$_{2}$PdAl$_{7}$Ge$_{4}$ down to 0.4 K. The small amount of entropy released in the magnetic state of Ce$_{2}$MAl$_{7}$Ge$_{4}$ (M = Co, Ir, Ni) and the reduced specific heat jump at $T_M$ suggest a strong Kondo interaction in these materials. Ce$_{2}$PdAl$_{7}$Ge$_{4}$ shows non-Fermi liquid behavior, possibly due to the presence of a nearby quantum critical point.
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