Quadrupolar susceptibility and magnetic phase diagram of PrNi2Cd20 with non-Kramers doublet ground state

ABSTRACT

In this study, ultrasonic measurements were performed on a single crystal of cubic PrNi₂Cd₂₀, down to a temperature of 0.02?K, to investigate the crystalline electric field ground state and search for possible phase transitions at low temperatures. The elastic constant (C₁₁?C₁₂)/2, which is related to the Γ₃-symmetry quadrupolar response, exhibits the Curie-type softening at temperatures below ～30?K, which indicates that the present system has a Γ₃ non-Kramers doublet ground state. A leveling-off of the elastic response appears below ～0.1?K toward the lowest temperatures, which implies the presence of level splitting owing to a long-range order in a finite-volume fraction associated with Γ₃-symmetry multipoles. A magnetic field–temperature phase diagram of the present compound is constructed up to 28?T for H || [110]. A clear acoustic de Haas–van Alphen signal and a possible magnetic-field-induced phase transition at H ～26?T are also detected by high-magnetic-field measurements.     

Ultrasound studies of single crystal thulium in an applied magnetic field

The paper reports the first measurements of the single crystal elastic constants of the heavy rare earth metal thulium as a function of temperature and magnetic field. The constants were obtained from ultrasonic velocity measurements over a temperature range of 4.2–296 K and in applied magnetic fields of up to 5 T. The elastic constants; C₁₁, C₃₃, C₄₄ and C₆₆=(C₁₁–C₁₂)/2 were determined from the ultrasonic velocities. Anomalies in the elastic constants were observed at 58 K from the c-axis propagated shear wave measurements and at 55 K from the c-axis propagated longitudinal wave measurements. Significant softening of the elastic constants C₃₃ and C₄₄ was observed close to T_N. Application of a magnetic field (>2 T) along the c-axis direction induced further softening of the material. Electromagnetic acoustic transducers (EMATs) were also employed in addition to conventional piezoelectric quartz transducers. A marked increase in the EMATs acoustic coupling efficiency (generation and detection efficiency) occurred close to T_N.     

Heat generation ability in AC magnetic field of nano MgFe2O4-based ferrite powder prepared by bead milling

Nanosized MgFe₂O₄-based ferrite powder having heat generation ability in an AC magnetic field was prepared by bead milling and studied for thermal coagulation therapy applications. The crystal size and the particle size significantly decreased by bead milling. The heat generation ability in an AC magnetic field improved with the milling time, i.e. a decrease in crystal size. However, the heat generation ability decreased for excessively milled samples with crystal sizes of less than 5.5 nm. The highest heat ability (ΔT=34 °C) in the AC magnetic field (370 kHz, 1.77 kA/m) was obtained for fine MgFe₂O₄ powder having a ca. 6 nm crystal size (the samples were milled for 6-8 h using 0.1 mm ? beads). The heat generation of the samples was closely related to hysteresis loss, a B-H magnetic property. The reason for the high heat generation properties of the samples milled for 6-8 h using 0.1 mm ? beads was ascribed to the increase in hysteresis loss by the formation of a single domain. Moreover, the improvement in heating ability was obtained by calcination of the bead-milled sample at low temperature. In this case, the maximum heat generation (ΔT=41 °C) ability was obtained for a ca. 11 nm crystal size sample was prepared by crystal growth during the sample calcination. On the other hand, the ΔT value for Mg_0.5Ca_0.5Fe₂O₄ was synthesized using a reverse precipitation method decreased by bead milling.     

Structural, magnetic and electric properties of HoMnO3 films on SrTiO3(001)

HoMnO₃ films were grown on pure and Nb-doped SrTiO₃ (001) substrates by pulsed laser deposition. The films grew epitaxially with the c-axis along the substrate normal. Varying the deposition temperature between 650 and 850 °C did not significantly affect the structural and magnetic properties of the films, whereas growth in oxygen partial pressures below 0.01 mbar lead to a degradation of the structural properties. Some of the films had a ferromagnetic-like magnetic phase transition at about 45 K, probably related to Mn₃O₄ precipitates; this magnetic response was isotropic. The Ho sublattice was found to be paramagnetic down to 5 K, but showing a pronounced anisotropy with the c-axis being the hard axis. The films showed a distinct dielectric anomaly at 16 K that depended on voltage and slightly on frequency in the range between 1 kHz and 1 MHz. The magnetoelectric effect was large with an in-plane field of 8 T suppressing the dielectric anomaly completely.     

Superparamagnetism and spin-glass like state for the MnFe2O4 nano-particles synthesized by the thermal decomposition method

MnFe₂O₄ nano-particles with an average size of about 7 nm were synthesized by the thermal decomposition method. Based on the magnetic hysteresis loops measured at different temperatures the temperature-dependent saturation magnetization (M_S) and coercivity (H_C) are determined. It is shown that above 20 K the temperature-dependence of the M_S and H_C indicates the magnetic behaviors in the single-domain nano-particles, while below 20 K, the change of the M_S and H_C indicates the freezing of the spin-glass like state on the surfaces. By measuring the magnetization–temperature (M–T) curves under the zero-field-cooling (ZFC) and field-cooling procedures at different applied fields, superparamagnetism behavior is also studied. Even though in the ZFC M–T curves peaks can be observed below 160 K, superparamagnetism does not appear until the temperature goes above 300 K, which is related with the strong inter-particle interaction.     

Elastic,magnetic, and magnetoelectric properties of the CaBaCo<Subscript>4</Subscript>O<Subscript>7</Subscript> multiferroic

The structural, elastic, magnetic, and magnetoelectric properties of the CaBaCo₄O₇ multiferroic are experimentally studied and compared with the properties of the related YBaCo₄O₇ cobaltite, where Y³⁺ ions substitute for Ca²⁺ ions. Unlike the frustrated YBaCo₄O₇ magnet, the softening of Young’s modulus and the hysteresis in the ΔE(T)/E ₀ curve of ferrimagnetic CaBaCo₄O₇ in the paramagnetic region are weak, and the anomaly during the magnetic transition increases by almost an order of magnitude. This difference can point to different characters of the development of a long-range magnetic order in these two cobaltites. The distortion of the crystal structure that removes the frustrations of exchange interactions is found to correlate with the magnetic behavior of the cobaltites under study. The magnetization curves of the Ca cobaltite have two steps below 15 K, which can point to the presence of a metastable state in a high magnetic field. The study of the longitudinal and transverse magnetoelectric effects in a pulsed magnetic field demonstrates that their magnitudes are maximal near T _C and change their character from linear to quadratic during passage through this temperature.     

The second-order elastic constants of AgBr from 77 to 300 K

The three independent second-order elastic constants of AgBr have been measured from room temperature down to liquid nitrogen temperature A single crystal with a (110) axis was used for the measurements The measured longitudinal elastic constant C'₁₁ = (C₁₁ + C₁₂ + 2C₄₄)/2 increases by 16% over this temperature range The elastic shear constant C₄₄) increases by almost 11%, while the elastic shear constant C' = (C₁₁ ? C₁₂)/2 increases by 50% over this range The measured bulk modulus B = (C₁₁) + 2C₁₂)/3 increases by almost 15% as the lattice becomes stiffer The initial temperature derivatives of the elastic constants are similar to those previously measured The changes in the elastic constants are basically linear down to approximately 150 K, where the temperature derivatives begin to decrease in magnitude These results are similar to those previously obtained for AgCl     

Adiabatic elastic moduli in ZnSe : Mn<Superscript>2+</Superscript> and ZnSe : V<Superscript>2+</Superscript> crystals

The temperature dependences of the elastic moduli C ₄₄ (C ₁₁ ? C ₁₂)/2 and C _l = (C ₁₁ + C ₁₂ + 2C ₄₄)/2 of ZnSe : V²⁺ (impurity concentration, 6 × 10¹⁸ cm^?3) and ZnSe : Mn²⁺ (9.4 × 10²⁰ cm^?3) are measured in the temperature range 1.4–100.0 K at frequencies of 52 and 156 MHz. The temperature dependences of the adiabatic elastic moduli are derived. It is established that softening of the symmetry modules is observed only in the crystal with an impurity having orbitally degenerate states.     

Dielectric and optical behaviors in relaxor ferroelectric Pb(In1/2Nb1/2)1−xTixO3 crystal

Dielectric permittivities (ε′,ε″) have been measured as functions of temperature (140-535 K) and frequency (500 Hz-2.0 MHz) in a (001)-cut Pb(In_1/2Nb_1/2)_0.7Ti_0.3O₃ (PINT30%) single crystal grown by the modified Bridgman method with Pb(Mg_1/3Nb_2/3)_0.71Ti_0.29O₃ (PMNT29%) seed crystal. A diffused phase transition was observed in the temperature region of ∼430-460 K with strong frequency dispersion. Above the Burns temperature T_B≅510 K, the dielectric permittivity was found to follow the Curie-Weiss behavior, ε′=C/(T−T_C), with parameters C=3.9×10⁵ and T_C=472 K. Below T_B≅510 K, polar nanoclusters are considered to appear and are responsible for the diffused dielectric anomaly. Optical transmission, refractive indices, and the Cauchy equations were obtained as a function of wavelength at room temperature. The unpoled crystal shows almost no birefringence, indicating that the average structural symmetry is optically isotropic. The crystal exhibits a broad transparency in the wavelength range of ∼0.4-6.0 μm.     

Effect of magnetic field on Nd0.7Pb0.3MnO3 single crystal

Magnetization and specific heat of Nd_0.7Pb_0.3MnO₃ single crystal are studied at applied magnetic field. Magnetization measurement at 0.3 T shows ferromagnetic phase below 150 K (T_C) and below 20 K displays an antiferromagnetic component. The latter appears to be destroyed at 4.8 T. This anomalous increase below 50 K is probably due to reorientation of Nd moments at high magnetic field. Heat capacity has been measured at 0-10 T at low temperature. The data have been fitted to contributions from free electrons (γ), ferromagnetic spin excitations (β_3/2), lattice and a Schottky-like anomaly related to the rare-earth magnetism of the Nd ions. Fitting yields that β_3/2 term is very small at 6 and 10 T because of introducing paramagnetic component in ferromagnetic phase at applied magnetic field. Peak due to Schottky anomaly is observed to be broadened with application of magnetic field and the magnitude of Schottky gap(Δ_Sch) also increases accordingly.     

Crystal structural, magnetic and electrical transport properties of CeKFeMoO6 double perovskite

The crystal structural, magnetic and electrical transport properties of double perovskite CeKFeMoO₆ have been investigated. The crystal structure of the compound is assigned to the monoclinic system with space group P2₁/n and its lattice parameters are a=0.55345(3) nm, b=0.56068(2) nm, c=0.78390(1) nm, β=89.874(2). The divergence between zero-field-cooling and field-cooling M-T curves demonstrates the anisotropic behavior. The Curie temperature measured from C_p-T curve is about 340 K. Isothermal magnetization curve shows that the saturation and spontaneous magnetization are 1.90 and 1.43 μ_B/f.u. at 300 K, respectively. The electrical behavior of the sample shows a semiconductor. The electrical transport behavior can be described by variable range hopping model. Large magnetoresistance, −0.88 and −0.18, can be observed under low magnetic field, 0.5 T, at low and room temperature, respectively.     

Elastic and electronic properties of YNi2B2C under pressure from first principles

The elastic and electronic structure properties of YNi₂B₂C under pressure are investigated by performing the generalized gradient approximation (GGA) and local density approximation (LDA) correction scheme in the frame of density functional theory (DFT). The pressure dependences of the normalized lattice parameters a/a₀ and c/c₀, the ratio c/a, and the normalized primitive volume V/V₀ of YNi₂B₂C are also obtained. The lattice constants and bulk modulus obtained are in agreement with the available experimental and other theoretical data. We have also studied the pressure dependences of elastic properties. It is found that, as pressure increases, the elastic constants C₁₁, C₃₃, C₆₆, C₁₂, and C₁₃ increase, the variation of elastic constant C₄₄ is not obvious. Moreover, our compressional and shear wave velocities V_L=6.99 km/s and V_S=3.67 km/s as well as the Debye temperature Θ=549.7 K at 0 GPa compare favorably with the available experimental data. The pressure dependences of band structures, energy gap and density of states are also investigated.     

Magnetocaloric properties in the Cr-doped La0.7Sr0.3MnO3 manganites

Single-phase polycrystalline samples of La_0.7Sr_0.3Mn_1-xCr_xO₃ with nominal composition of x=0.00, 0.20, 0.40 and 0.50 were prepared by a conventional solid-state reaction method in air. Investigations of magnetization were carried out in the temperature range 5-400 K and magnetic field range 0-8 T. It was found that the Curie temperature T_C decreases with increasing x and the maximum magnetic entropy change (−ΔS_M) for x=0.20 is ∼1.203 and ∼2.653 J/kg K, respectively for 2 and 6 T magnetic field near the temperature of 280 K.     

Magnetic measurements on single crystals of Ho(CF3SO3)3.9H2O and crystal field investigation

Magnetic measurements on single crystals of holmium trifluoromethanesulfonate (HoTFMS) have been carried out from 300 to 12.5 K. The hexagonal crystal structure of HoTFMS is very similar to that of the hydrated rare earth ethylsulfates with the non-Kramers Ho³⁺ ion occupying a site of C_3h symmetry. A very good theoretical simulation of the principal magnetic susceptibilities, observed by us and the Friedberg group, over the wide range 300 to ∼1.0 K was obtained with the crystal field J-mixed eigenvectors taking into consideration intermediate coupling effects. No ordering effects were noticed by us down to ∼12.5 K indicating the interionic interaction to be of predominantly dipolar type consistent with the discovery of a ferromagnetic transition at T∼0.23 K by the Friedberg group. The g-values are found to be in reasonable agreement with those derived from other sources. The Schottky anomaly in the electronic heat capacity observed at ∼6 K by the Friedberg group is borne out excellently by our theoretical values computed from the crystalline Stark pattern. The thermal behavior of quadrupole splitting and hyperfine heat capacity is calculated and our computed values explain very well the principal anomaly in C_N observed experimentally.     

The effect of different temperature annealing on phase relation of LaFe11.5Si1.5 and the magnetocaloric effects of La0.8Ce0.2Fe11.5−xCoxSi1.5 alloys

The phase relation of LaFe_11.5Si_1.5 alloys annealed at different high-temperature from 1223 K (5 h) to 1673 K (0.5 h) has been studied. The powder X-ray diffraction (XRD) patterns show that large amount of 1:13 phase begins to form in the matrix alloy consisting of α-Fe and LaFeSi phases when the annealing temperature is 1423 K. In the temperature range from 1423  to 1523 K, α-Fe and LaFeSi phases rapidly decrease to form 1:13 phase, and LaFeSi phase is rarely observed in the XRD pattern of LaFe_11.5Si_1.5 alloy annealed at 1523 K. With annealing temperature increasing from 1573  to 1673 K, the LaFeSi phase is detected again in the LaFe_11.5Si_1.5 alloy, and there is La₅Si₃ phase when the annealing temperature reaches 1673 K. There almost is no change in the XRD patterns of LaFe_11.5Si_1.5 alloys annealed at 1523 K for 3-5 h. According to this result, the La_0.8Ce_0.2Fe_11.5−xCo_xSi_1.5 (0≤×≤0.7) alloys are annealed at 1523 K (3 h). The analysis of XRD patterns shows that La_0.8Ce_0.2Fe_11.5xCo_xSi_1.5 alloys consist of the NaZn₁₃-type main phase and α-Fe impurity phase. With the increase of Co content from x=0 to 0.7, the Curie temperature T_C increases from 180 to 266 K. Because the increase of Co content can weaken the itinerant electron metamagnetic transition, the order of the magnetic transition at T_C changes from first to second-order between x=0.3 and 0.5. Although the magnetic entropy change decreases from 34.9 to 6.8 J/kg K with increasing Co concentration at a low magnetic field of 0-2 T, the thermal and magnetic hysteresis loss reduces remarkably, which is very important for the magnetic refrigerant near room temperature.     

Shape- and field-dependent Morin transitions in structured α-Fe2O3

We report shape- and field-dependent magnetic properties of ellipsoid-, spindle-, flattened- and rhombohedra-shaped α-Fe₂O₃ samples prepared by solvothermal technique. We observed that a magnetic spin-flip mechanism, mostly known as Morin transition (T_M), depends on the shape of α-Fe₂O₃ as well as on the applied magnetic field. In each of these structures the obtained value of T_M was less than its bulk value of 263 K. We observed that T_M shifted from highest 251.4 K for ellipsoid to lowest 220.8 K for rhombohedra structure, with intermediate values of T_M for the other two structures. However, for rhombohedra structure T_M shifted from 220.8 to 177.5 K under the external magnetic field of 100 Oe-30 kOe, respectively. The observed lowering of T_M in the structured sample was analyzed in terms of elementary size, shape of the nanocrystallites, lattice parameters and occupancy of Fe⁺³ ions as well. These parameters were determined from the Rietveld refinement process using MAUD software.     

Self-, N2- and O2-broadening coefficients for the CO2 transitions near-IR measured by a diode laser photoacoustic spectrometer

Using a high-resolution tunable diode laser photoacoustic spectrometer, self-, N₂ and O₂ pressure broadening coefficients for the first 11 transitions of ¹²C¹⁶O₂ in the R branch of the (30012) ← (00001) overtone band at the 6348 cm⁻¹ have been revisited at room temperature (∼298 K). Air-broadening parameters have also been calculated from the N₂ and O₂ measurements. The dependence of the broadening on rotational quantum number m is discussed. The recorded lineshapes are fitted with standard Voigt line profiles in order to determine the collisional broadening coefficients of carbon dioxide transitions. The results are compared to our previous measurements and to the values reported in the HITRAN04 database and by other research group with a different spectroscopic technique.     

Magnetocrystalline anisotropy in RAu2Ge2 (R = La, Ce and Pr) single crystals

Anisotropic magnetic properties of single crystalline RAu₂Ge₂ (R=La, Ce and Pr) compounds are reported. LaAu₂Ge₂ exhibits a Pauli-paramagnetic behaviour whereas CeAu₂Ge₂ and PrAu₂Ge₂ show an antiferromagnetic ordering with Nèel temperatures T_N = 13.5 and 9 K, respectively. The anisotropic magnetic response of Ce and Pr compounds establishes [0 0 1] as the easy axis of magnetization and a sharp spin-flip type metamagnetic transition is observed in the magnetic isotherms with H // [0 0 1]. The transport and magnetotransport behaviour of these compounds, in particular LaAu₂Ge₂, indicate an anisotropic Fermi surface. The magnetoresistivity of CeAu₂Ge₂ apparently reveals the presence of a residual Kondo interaction. A crystal electric field analysis of the anisotropic susceptibility in conjunction with the experimentally inferred Schottky heat capacity enables us to propose a crystal electric field level scheme for Ce and Pr compounds. For CeAu₂Ge₂ our values are in excellent agreement with the previous reports on neutron diffraction. The heat capacity data in LaAu₂Ge₂ show clearly the existence of Einstein contribution to the heat capacity.     

Study on dielectric and magnetic properties of Ho3Fe5O12 ceramics

Ho₃Fe₅O₁₂ ceramics with garnet structure were prepared by the solid-state reaction method. The results revealed the existence of Fe²⁺ ions have intensive influence on dielectric and magnetic properties of Ho₃Fe₅O₁₂ ceramics, which could be further confirmed by oxygen treatment. With a magnetic field lower than 10 kOe, the ME coefficient reaches 33 ps m⁻¹ at room temperature. And the ME coupling was further verified by dielectric anomaly near Néel temperature.     

High heat generation ability in AC magnetic field for nano-sized magnetic Y3Fe5O12 powder prepared by bead milling

Nano-sized magnetic Y₃Fe₅O₁₂ ferrite having a high heat generation ability in an AC magnetic field was prepared by bead milling. A commercial powder sample (non-milled sample) of ca. 2.9 μm in particle size did not show any temperature enhancement in the AC magnetic field. The heat generation ability in the AC magnetic field improved with a decrease in the average crystallite size for the bead-milled Y₃Fe₅O₁₂ ferrites. The highest heat ability in the AC magnetic field was for the fine Y₃Fe₅O₁₂ powder with a 15-nm crystallite size (the samples were milled for 4 h using 0.1 mm? beads). The heat generation ability of the excessively milled Y₃Fe₅O₁₂ samples decreased. The main reason for the high heat generation property of the milled samples was ascribed to an increase in the Néel relaxation of the superparamagnetic material. The heat generation ability was not influenced by the concentration of the ferrite powder. For the samples milled for 4 h using 0.1 mm? beads, the heat generation ability (W g⁻¹) was estimated using a 3.58×10⁻⁴ fH² frequency (f/kHz) and the magnetic field (H/kA m⁻¹), which is the highest reported value of superparamagnetic materials.