No Arabic abstract
The series of intermetallic compounds $R$NiSi$_3$ ($R$ = rare earth) shows interesting magnetic properties evolving with $R$ and metamagnetic transitions under applied magnetic field for some of the compounds. The microscopic magnetic structures must be determined to rationalize such rich behavior. Here, resonant x-ray magnetic diffraction experiments are performed on single crystals of GdNiSi$_{3}$ and TbNiSi$_{3}$ at zero field. The primitive magnetic unit cell matches the chemical cell below the Neel temperatures $T_{N}$ = 22.2 and 33.2 K, respectively. The magnetic structure is determined to be the same for both compounds (magnetic space group $Cmmm$). It features ferromagnetic {it ac} planes that are stacked in an antiferromagnetic $+-+-$ pattern, with the rare-earth magnetic moments pointing along the $vec{a}$ direction, which contrasts with the $+--+$ stacking and moment direction along the $vec{b}$ axis previously reported for YbNiSi$_3$. This indicates a sign reversal of the coupling constant between second-neighbor $R$ planes as $R$ is varied from Gd and Tb to Yb. The long {it b} lattice parameter of GdNiSi$_{3}$ and TbNiSi$_{3}$ shows a magnetoelastic expansion upon cooling below $T_N$, pointing to the conclusion that the $+-+-$ stacking is stabilized under lattice expansion. A competition between distinct magnetic stacking patterns with similar exchange energies tuned by the size of $R$ sets the stage for the magnetic ground state instability observed along this series.
We carried out detailed studies of the magnetic structure, magnetoelastic coupling, and thermal properties of EuCrO$_3$ nano-powders from room temperature to liquid helium temperature. Our neutron powder diffraction and X-ray powder diffraction measurements provide precise atomic positions of all atoms in the cell, especially for the light oxygen atoms. The low-temperature neutron powder diffraction data revealed extra Bragg peaks of magnetic origin which can be attributed to a $G_x$ antiferromagnetic structure with an ordered moment of $sim$ 2.4 $mu_{rm B}$ consistent with the $3d^3$ electronic configuration of the Cr$^{3+}$ cations. Apart from previously reported antiferromagnetic and ferromagnetic transitions in EuCrO$_3$ at low temperatures, we also observed an anomaly at about 100 K. This anomaly was observed in temperature dependence of samples, lattice parameters, thermal expansion, Raman spectroscopy, permittivity and conductance measurements. This anomaly is attributed to the magnetoelastic distortion in the EuCrO$_3$ crystal.
The Co2V2O7 is recently reported to exhibit amazing magnetic field-induced magnetization plateaus and ferroelectricity, but its magnetic ground state remains ambiguous due to its structural complexity. Magnetometry measurements, and time-of-flight neutron powder diffraction (NPD) have been employed to study the structural and magnetic properties of Co2V2O7, which consists of two non-equivalent Co sites. Upon cooling below the Neel temperature TN = 6.3 K, we observe magnetic Bragg peaks at 2K in NPD which indicated the formation of long range magnetic order of Co2+ moments. After symmetry analysis and magnetic structure refinement, we demonstrate that Co2V2O7 possesses a complicated non-collinear magnetic ground state with Co moments mainly located in b-c plane and forming a non-collinear spin-chain-like structure along the c-axis. The ab initio calculations demonstrate that the non-collinear magnetic structure is more stable than various ferromagnetic states at low temperature. The non-collinear magnetic structure with canted up-up-down-down spin configuration is considered as the origin of magnetoelectric coupling in Co2V2O7 because the inequivalent exchange striction induced by the spin-exchange interaction between the neighboring spins is the driving force of ferroelectricity. Besides, it is found that the deviation of lattice parameters a and b is opposite below TN, while the lattice parameter c and stay almost constant below TN, evidencing the anisotropic magnetoelastic coupling in Co2V2O7.
High-quality single crystals of CoTiO$_3$ are grown and used to elucidate in detail structural and magnetostructural effects by means of high-resolution capacitance dilatometry studies in fields up to 15 T which are complemented by specific heat and magnetization measurements. In addition, we refine the single-crystal structure of the ilmenite ($Rbar{3}$) phase. At the antiferromagnetic ordering temperature $T_mathrm{N}$, pronounced $lambda$-shaped anomaly in the thermal expansion coefficients signals shrinking of both the $c$ and $b$ axes, indicating strong magnetoelastic coupling with uniaxial pressure along $c$ yielding six times larger effect on $T_mathrm{N}$ than the pressure applied in-plane. The hydrostatic pressure dependency derived by means of Gruneisen analysis amounts to $partial T_mathrm{N}/ partial papprox 2.7(4)$~K/GPa. The high-field magnetization studies in static and pulsed magnetic fields up to 60~T along with high-field thermal expansion measurements facilitate in constructing the complete anisotropic magnetic phase diagram of CoTiO$_3$. While the results confirm the presence of significant magnetodielectric coupling, our data show that magnetism drives the observed structural, dielectric, and magnetic changes both in the short-range ordered regime well-above $T_mathrm{N}$ as well as in the long-range magnetically ordered phase.
We report high-resolution capacitance dilatometry studies on the uniaxial length changes in a NdB$_4$ single crystal. The evolution of magnetically ordered phases below $T_{rm N}$= 17.2~K (commensurate antiferromagnetic phase, cAFM), $T_{rm IT}$= 6.8~K (intermediate incommensurate phase, IT), and $T_{rm LT}$= 4.8~K (low-temperature phase, LT) is associated with pronounced anomalies in the thermal expansion coefficients. The data imply significant magneto-elastic coupling and evidence of a structural phase transition at $T_{rm LT}$ . While both cAFM and LT favor structural anisotropy $delta$ between in-plane and out-of-plane length changes, it competes with the IT-type of order, i.e., $delta$ is suppressed in that phase. Notably, finite anisotropy well above $T_{rm N}$ indicates short-range correlations which are, however, of neither cAFM, IT, nor LT-type. Gruneisen analysis of the ratio of thermal expansion coefficient and specific heat enables the derivation of uniaxial as well as hydrostatic pressure dependencies. While $alpha$/$c_{rm p}$ evidences a single dominant energy scale in LT, our data imply precursory fluctuations of a competing phase in IT and cAFM, respectively. Our results suggest the presence of orbital degrees of freedom competing with cAFM and successive evolution of a magnetically and orbitally ordered ground state.
We have studied the crystal and magnetic structures of Fe-doped hexagonal manganites LuMn1-xFexO3 (x = 0, 0.1, 0.2, and 0.3) by using bulk magnetization and neutron powder diffraction methods. The samples crystalize consistently in a hexagonal structure and maintain the space group P63cm from 2 to 300 K. The Neel temperature TN increases continuously with increasing Fe-doping. In contrast to a single {Gamma}4 representation in LuMnO3, the magnetic ground state of the Fe-doped samples can only be described with a spin configuration described by a mixture of {Gamma}3 (P63cm) and {Gamma}4 (P63cm) representations, whose contributions have been quantitatively estimated. The drastic effect of Fe-doping is highlighted by composition-dependent spin reorientations. A phase diagram of the entire composition series is proposed based on the present results and those reported in literature. Our result demonstrates the importance of tailoring compositions in increasing magnetic transition temperatures of multiferroic systems.