The role of hyperfine coupling in magnetic and quadrupolar ordering of Pr3Pd20Si6

We study the ternary clathrate Pr3Pd20Si6 in specific heat and AC-susceptibility measurements on a high-quality single crystal, distinguishing antiferromagnetic (AFM) and antiferroquadrupolar (AFQ) ordering on two sublattices of inequivalent Pr sites. The specific heat shows the direct involvement of nuclear spin degrees of freedom in the AFM ordering, which is well supported by our calculation of the hyperfine level scheme without adjustable parameters. Pr3Pd20Si6 is therefore one of the rare materials where the nuclear moments are involved in the formation of the magnetic ground state.Comment: 5 pages, 5 figure

Spiral magnetic structure in spin-5/2 frustrated trimerized chains in SrMn3P4O14

We study a spin-5/2 antiferromagnetic trimerized chain substance SrMn3P4O14 using neutron powder diffraction experiments. The coplanar spiral magnetic structure appears below T_N1 = 2.2(1) K. Values of several magnetic structure parameters change rapidly at T_N2 = 1.75(5) K, indicating another phase transition, although the magnetic structures above and below T_N2 are the qualitatively same. The spiral magnetic structure can be explained by frustration between nearest-neighbor and next-nearest-neighbor exchange interactions in the trimerized chains.Comment: submitted to Phys. Rev.

Negative magnetization of Li2Ni2Mo3O12 having a spin system composed of distorted honeycomb lattices and linear chains

We study themagnetism of a spin-1 substance Li2Ni2Mo3O12. The spin system consists of distorted honeycomb lattices and linear chains of Ni2+ spins. Li+ ions enter about 25% and 50% of the honeycomb and chain Ni sites, respectively, creating disorder in both spin subsystems. A magnetic phase transition occurs at Tc = 8.0 K in the zero magnetic field. In low magnetic fields, the magnetization increases rapidly below Tc, decreases below 7 K, and finally becomes negative at low temperatures. We determine the magnetic structure using neutron powder diffraction results. The honeycomb lattices and linear chains show antiferromagnetic and ferromagnetic long-range order, respectively. We investigate static and dynamic magnetic properties using the local probe technique of muon spin relaxation. We discuss the origin of the negative magnetization

Evidence for Large Electric Polarization From Collinear Magnetism in TmMnO\u3csub\u3e3\u3c/sub\u3e

There has been tremendous research activity in the field of magneto-electric (ME) multiferroics after Kimura et al (2003 Nature 426 55) showed that antiferromagnetic and ferroelectric orders coexist in orthorhombically distorted perovskite TbMnO3 and are strongly coupled. It is now generally accepted that ferroelectricity in TbMnO3 is induced by magnetic long-range order that breaks the symmetry of the crystal and creates a polar axis (Kenzelmann et al 2005 Phys. Rev. Lett. 95 087206). One remaining key question is whether magnetic order can induce ferroelectric polarization that is as large as that of technologically useful materials. We show that ferroelectricity in orthorhombic (o) TmMnO3 is induced by collinear magnetic order, and that the lower limit for its electric polarization is larger than in previously investigated orthorhombic heavy rare-earth manganites. The temperature dependence of the lattice constants provides further evidence of large spin–lattice coupling effects. Our experiments suggest that the ferroelectric polarization in the orthorhombic perovskites with commensurate magnetic ground states could pass the 1 μC cm-2 threshold, as predicted by theory (Sergienko et al 2006 Phys. Rev. Lett. 97 227204; Picozzi et al 2007 Phys. Rev. Lett. 99 227201)

Ferroquadrupole ordering and Gamma_5 rattling motion in clathrate compound Ce_3Pd_20Ge_6

Lattice effects in a cerium based clathrate compound Ce_3Pd_20Ge_6 with a cubic Cr_23C_6-type structure have been investigated by ultrasonic and thermal expansion measurements. Elastic softenings of (C_11-C_12)/2 and C_44 proportional to the reciprocal temperature 1/T above T_Q1 = 1.25 K are well described in terms of the quadrupole susceptibility for the ground state Gamma_8 quartet. A huge softening of 50 % in (C_11-C_12)/2 and a spontaneous expansion DL/L = 1.9x10^-4 along the [001] direction in particular indicate the ferroquadrupole ordering of O_2^0 below T_Q1. The elastic anomalies associated with the antiferromagnetic ordering at T_N2 = 0.75 K and the incommensurate antiferromagnetic ordering are also found. Notable frequency dependence of C_44 around 10 K is accounted for by the Debye-type dispersion indicating a Gamma_5 rattling motion of an off-center Ce ion along the [111] direction with eight fractionally occupied positions around the 4a site in a cage. The thermally activated Gamma_5 rattling motion obeying a relaxation time t = t_0exp(E/k_BT) with an attempt time t_0 = 3.1x10^-11 sec and an activation energy E = 70 K dies out with decreasing temperature, and then the off-center tunneling state of Ce ion in the 4a-site cage will appear at low temperatures.Comment: 11 pages, 15 figures, to be published on Phys. Rev.

Ferrimagnetic Ordering and Spin-Glass State in Diluted GdFeO₃-Type Perovskites (Lu_0.5Mn_0.5)(Mn_1−<i>x</i>Ti<i>_x</i>)O₃ with <i>x</i> = 0.25, 0.50, and 0.75

ABO3 perovskite materials with small cations at the A site, especially those with ordered cation arrangements, have attracted a great deal of interest because they show unusual physical properties and deviations from the general characteristics of perovskites. In this work, perovskite solid solutions (Lu0.5Mn0.5)(Mn1−xTix)O3 with x = 0.25, 0.50, and 0.75 were synthesized by means of a high-pressure, high-temperature method at approximately 6 GPa and approximately 1550 K. All the samples crystallize in the GdFeO3-type perovskite structure (space group Pnma) and have random distributions of the small Lu3+ and Mn2+ cations at the A site and Mn4+/3+/2+ and Ti4+ cations at the B site, as determined by Rietveld analysis of high-quality synchrotron X-ray powder diffraction data. Lattice parameters are a = 5.4431 Å, b = 7.4358 Å, c = 5.1872 Å (for x = 0.25); a = 5.4872 Å, b = 7.4863 Å, c = 5.2027 Å (for x = 0.50); and a = 5.4772 Å, b = 7.6027 Å, c = 5.2340 Å (for x = 0.75). Despite a significant dilution of the A and B sublattices by non-magnetic Ti4+ cations, the x = 0.25 and 0.50 samples show long-range ferrimagnetic order below TC = 89 K and 36 K, respectively. Mn cations at both A and B sublattices are involved in the long-range magnetic order. The x = 0.75 sample shows a spin-glass transition at TSG = 6 K and a large frustration index of approximately 22. A temperature-independent dielectric constant was observed for x = 0.50 (approximately 32 between 5 and 150 K) and for x = 0.75 (approximately 50 between 5 and 250 K)