Magnetoelectric properties of A2A_2[FeCl5_5(H2_2O)] with A=A = K, Rb, Cs

The compounds $A_2$[FeCl$_5$(H$_2$O)] with $A=$ K, Rb, Cs are identified as new linear magnetoelectric materials. We present a detailed investigation of their linear magnetoelectric properties by measurements of pyroelectric currents, dielectric constants and magnetization. The anisotropy of the linear magnetoelectric effect of the K-based and Rb-based compound is consistent with the magnetic point group $m'm'm'$, already reported in literature. A symmetry analysis of the magnetoelectric effect of the Cs-based compound allows to determine the magnetic point group $mmm'$ and to develop a model for its magnetic structure. In addition, magnetic-field versus temperature phase diagrams are derived and compared to the closely related multiferroic (NH$_4$)$_2$[FeCl$_5$(H$_2$O)].Comment: 17 pages, 10 figures (updated to the weakly revised version that has been accepted for publication

Anisotropy study of multiferroicity in the pyroxene NaFeGe2_2O6_6

We present a study of the anisotropy of the dielectric, magnetic and magnetoelastic properties of the multiferroic clinopyroxene NaFeGe$_2$O$_6$. Pyroelectric currents, dielectric constants and magnetic susceptibilities as well as the thermal expansion and the magnetostriction were examined on large synthetic single crystals of NaFeGe$_2$O$_6$. The spontaneous electric polarization detected below $T_{\rm C}\simeq 11.6$ K in an antiferromagnetically ordered state ($T_{\rm N}\simeq 13$ K) is mainly lying within the $ac$ plane with a small component along $b$, indicating a triclinic symmetry of the multiferroic phase of NaFeGe$_2$O$_6$. The electric polarization can be strongly modified by applying magnetic fields along different directions. We derive detailed magnetic-field versus temperature phase diagrams and identify three multiferroic low-temperature phases, which are separated by a non-ferroelectric, antiferromagnetically ordered state from the paramagnetic high-temperature phase.Comment: 14 pages, 8 figures. (minor modifications and corrections of the text

Kinetics of the Multiferroic Switching in MnWO4_4

The time dependence of switching multiferroic domains in MnWO$_4$ has been studied by time-resolved polarized neutron diffraction. Inverting an external electric field inverts the chiral magnetic component within rise times ranging between a few and some tens of milliseconds in perfect agreement with macroscopic techniques. There is no evidence for any faster process in the inversion of the chiral magnetic structure. The time dependence is well described by a temperature-dependent rise time suggesting a well-defined process of domain reversion. As expected, the rise times decrease when heating towards the upper boundary of the ferroelectric phase. However, switching also becomes faster upon cooling towards the lower boundary, which is associated with a first-order phase transition

Muon-spin relaxation and heat capacity measurements on the magnetoelectric and multiferroic pyroxenes LiFeSi2O6 and NaFeSi2O6

The results of muon-spin relaxation and heat capacity measurements on two pyroxene compounds LiFeSi2O6 and NaFeSi2O6 demonstrate that despite their underlying structural similarity the magnetic ordering is considerably different. In LiFeSi2O6 a single muon precession frequency is observed below TN, consistent with a single peak at TN in the heat capacity and a commensurate magnetic structure. In applied magnetic fields the heat capacity peak splits in two. In contrast, for natural NaFeSi2O6, where multiferroicity has been observed in zero-magnetic-field, a rapid Gaussian depolarization is observed showing that the magnetic structure is more complex. Synthetic NaFeSi2O6 shows a single muon precession frequency but with a far larger damping rate than in the lithium compound. Heat capacity measurements reproduce the phase diagrams previously derived from other techniques and demonstrate that the magnetic entropy is mostly associated with the build up of correlations in the quasi-one-dimensional Fe3+ chains

Low-temperature ordered phases of the spin-12\frac{1}{2} XXZ chain system Cs2_2CoCl4_4

In this study the magnetic order of the spin-1/2 XXZ chain system Cs$_2$CoCl$_4$ in a temperature range from 50 mK to 0.5 K and in applied magnetic fields up to 3.5 T is investigated by high-resolution measurements of the thermal expansion and the specific heat. Applying magnetic fields along a or c suppresses $T_\textrm{N}$ completely at about 2.1 T. In addition, we find an adjacent intermediate phase before the magnetization saturates close to 2.5 T. For magnetic fields applied along b, a surprisingly rich phase diagram arises. Two additional transitions are observed at critical fields $\mu_0 H_{SF1}\simeq 0.25$ T and $\mu_0 H_{SF2}\simeq 0.7$ T, which we propose to arise from a two-stage spin-flop transition.Comment: 10 pages, 10 figure

Electronic excitations in 5d45d^4 J=0 Os4+^{4+} halides studied by RIXS and optical spectroscopy

We demonstrate that the cubic antifluorite-type halides K$_2$OsCl$_6$, K$_2$OsBr$_6$, and Rb$_2$OsBr$_6$ are excellent realizations of non-magnetic J=0 compounds. The magnetic susceptibility shows the corresponding Van-Vleck type behavior and no sign of defects. We investigate the electronic excitations with two complementary techniques, resonant inelastic x-ray scattering (RIXS) and optical spectroscopy. This powerful combination allows us to thoroughly study, e.g., on-site intra-$t_{2g}$ excitations and $t_{2g}$-to-$e_g$ excitations as well as inter-site excitations across the Mott gap and an exciton below the gap. In this way, we determine the electronic parameters with high accuracy, altogether yielding a comprehensive picture. In K$_2$OsCl$_6$, we find the spin-orbit coupling constant $\zeta$=0.34 eV, Hund's coupling $J_H$=0.43 eV, the onset of excitations across the Mott gap at $\Delta$=2.2 eV, the cubic crystal-field splitting 10Dq=3.3 eV, and the charge-transfer energy $\Delta_{CT}$=4.6 eV. With $J_H/\zeta$=1.3, K$_2$OsCl$_6$ is in the intermediate-coupling regime. In a $t_{2g}$-only Kanamori picture, the above values correspond to $\zeta^{eff}$=0.41 eV and $J_H^{eff}$=0.28 eV, which is very close to results reported for related $5d^4$ iridates. In the tetragonal phase at 5 K, the non-cubic crystal field causes a peak splitting of the J=1 state as small as 4 meV. Compared to K$_2$OsCl$_6$, the bromides K$_2$OsBr$_6$ and Rb$_2$OsBr$_6$ show about 12-14 % smaller values of 10Dq and $\Delta_{CT}$, while the spin-orbit-entangled intra-$t_{2g}$ excitations below 2 eV and hence $\zeta$ and $J_H$ are reduced by less than 4 %. Furthermore, the Mott gap in K$_2$OsBr$_6$ is reduced to about 1.8 eV.Comment: 14 pages, 14 figure

Annual Feedback Is an Effective Tool for a Sustained Increase in Calcium Intake among Older Women

We aimed to optimize calcium intake among the 2,000+ older women taking part in the Vital D study. Calcium supplementation was not included in the study protocol. Our hypothesis was that annual feedback of calcium intake and informing women of strategies to improve calcium intake can lead to a sustained increase in the proportion of women who consume adequate levels of the mineral. Calcium intake was assessed on an annual basis using a validated short food frequency questionnaire (FFQ). Supplemental calcium intake was added to the dietary estimate. Participants and their nominated doctor were sent a letter that the participant’s estimated daily calcium intake was adequate or inadequate based on a cutoff threshold of 800 mg/day. General brief statements outlining the importance of an adequate calcium intake and bone health were included in all letters. At baseline, the median daily consumption of calcium was 980 mg/day and 67 percent of 1,951 participants had calcium intake of at least 800 mg per day. Of the 644 older women advised of an inadequate calcium intake at baseline (<800 mg/day), 386 (60%) had increased their intake by at least 100 mg/day when re-assessed twelve months later. This desirable change was sustained at 24 months after baseline with almost half of these women (303/644) consuming over 800 mg calcium per day. This study devised an efficient method to provide feedback on calcium intake to over 2,000 older women. The improvements were modest but significant and most apparent in those with a low intake at baseline. The decreased proportion of these women with an inadequate intake of calcium 12- and 24-months later, suggests this might be a practical, low cost strategy to maintain an adequate calcium intake among older women