Gradual localization of 5f states in orthorhombic UTX ferromagnets - polarized neutron diffraction study of Ru substituted UCoGe

We report on a microscopic study of the evolution of ferromagnetism in the Ru substituted ferromagnetic superconductor (FM SC) UCoGe crystallizing in the orthorhombic TiNiSi-type structure. For that purpose, two single crystals with composition UCo0.97Ru0.03Ge and UCo0.88Ru0.12Ge have been prepared and characterized by magnetization, AC susceptibility, specific heat and electrical resistivity measurements. Both compounds have been found to order ferromagnetically below TC = 6.5 K and 7.5 K, respectively, which is considerably higher than the TC = 3 K of the parent compound UCoGe. The higher values of TC are accompanied by enhanced values of the spontaneous moment mspont. = 0.11 mB/f.u. and mspont. = 0.21 mB/f.u., respectively in comparison to the tiny spontaneous moment of UCoGe (about 0.07mB/f.u.). No sign of superconductivity was detected in either compound. The magnetic moments of the samples were investigated on the microscopic scale using polarized neutron diffraction (PND) and for UCo0.88Ru0.12Ge also by soft X-ray magnetic circular dichroism (XMCD). The analysis of the PND results indicates that the observed enhancement of ferromagnetism is mainly due to the growth of the orbital part of the uranium 5f moment mL(U), reflecting a gradual localization of the 5f electrons with Ru substitution. In addition, the parallel orientation of the U and Co moments has been established in both substituted compounds. The results are discussed and compared with related isostructural ferromagnetic UTX compounds (T - transition metals, X - Si, Ge) in the context of a varying degree of the 5f-ligand hybridization

H-Mediated magnetic interactions between layers in a 2D Mn-II-dicyanamide polymer: neutron diffraction, DFT, and quantum Monte Carlo calculations

We report neutron-diffraction investigations of the quasi-2D Mn-II(dca)(2)(pym)(H2O) (pym = N2C4H4) compound, where high-spin Mn-II ions are bridged by dicyanamide anions, [N(CN)(2)](-) (herein abbreviated dca). Inside the layers, Mn2+ ions are connected by single or double dca bridges. The magnetic phase diagram was established by neutron diffraction on a single crystal. In the low-field phase, the Mn-II ions are antiferromagnetically ordered in the layers, with moments nearly parallel to the c axis, and the layers are antiferromagnetically coupled. The spin-flop phase corresponds to ferromagnetic coupling between the antiferromagnetic layers, in which the Mn-II moments are nearly perpendicular to the c axis. The induced spin-density distribution in the paramagnetic phase, determined by polarized neutron diffraction, visualizes the superexchange pathways through the dca ligands within the layers and through H bonding between neighboring layers. The theoretical spin density obtained by bidimensional periodic DFT calculations is compared with the experimental results. Furthermore, quantum Monte Carlo simulations have been performed to compare the DFT results with experimental susceptibility measurements