No Arabic abstract
We have investigated the effects of substituting In for Mn on the antiferromagnetic phase transition in YMnO3 using magnetic, dielectric, and specific heat measurements. We prepared a set of isostructural phase pure hexagonal YMn$_{1-x}$In$_{x}$O$_{3}$ samples having x=0 to x=0.9, which exhibit a systematic decrease of the antiferromagnetic ordering temperature with increasing In content. The multiferroic phase, which develops below TN, appears to be completely suppressed for x$geq$0.5 in the temperature range investigated, which can be attributed solely to the dilution of magnetic interactions as the crystal structure remains hexagonal. Similar to previous reports, we find an enhancement of the magnetocapacitive coupling on dilution with non-magnetic ions.
We report an investigation of hexagonal Y_(1-x)Eu_xMnO_3 ceramics with x=0, 0.1 and 0.2 using infrared and THz spectroscopies in the temperature range between 5 and 900 K. The temperature dependence of the THz permittivity reveals a kink near the antiferromagnetic phase transition temperature T_N ~ 70 K giving evidence of a strong spin-lattice coupling. Below T_N two absorption peaks were revealed in the THz spectra close to 43 and 73 cm-1. While the first peak corresponds to a sharp antiferromagnetic resonance exhibiting softening on heating towards TN, the second one may be attributed to an impurity mode or a multiphonon absorption peak. High-temperature THz spectra measured up to 900 K reveal only small gradual increase of the permittivity in agreement with a weak phonon softening observed in the infrared reflectance spectra upon heating. This corresponds to an improper ferroelectric character of the phase transition proposed from first principle calculations by Fennie and Rabe [Phys. Rev. B 72 (2005), pp. 100103(R)].
Hexagonal LuFeO$_3$ has drawn a lot of research attention due to its contentious room-temperature multiferroicity. Due to the unstability of hexagonal phase in the bulk form, most experimental studies focused on LuFeO$_3$ thin films which can be stabilized by strain using proper substrates. Here we report on the hexagonal phase stabilization, magnetism, and magnetoelectric coupling of bulk LuFeO$_3$ by partial Sc-substitution of Lu. First, our first-principles calculations show that the hexagonal structure can be stabilized by partial Sc substitution, while the multiferroic properties including the noncollinear magnetic order and geometric ferroelectricity remain robustly unaffected. Therefore, Lu$_{1-x}$Sc$_x$FeO$_3$ can act as a platform to check the multiferroicity of LuFeO$_3$ and related materials in the bulk form. Second, the magnetic characterizations on bulk Lu$_{1-x}$Sc$_x$FeO$_3$ demonstrate a magnetic anomaly (probable antiferromagnetic ordering) above room temperature, $sim425-445$ K, followed by magnetic transitions in low temperatures ($sim167-172$ K). In addition, a magnetoelectric response is observed in the low temperature region. Our study provides useful information on the multiferroic physics of hexagonal $R$FeO$_3$ and related systems.
Dielectric and magnetic properties of Eu0.5Ba0.25Sr0.25TiO3 are investigated between 10 K and 300 K in the frequency range from 10 Hz to 100 THz. A peak in permittivity revealed near 130 K and observed ferroelectric hysteresis loops prove the ferroelectric order below thistemperature. The peak in permittivity is given mainly by softening of the lowest frequency polar phonon (soft mode revealed in THz and IR spectra) that demonstrates displacive character of the phase transition. Room-temperature X-ray diffraction analysis reveals cubic structure, but the IR reflectivity spectra give evidence of a lower crystal structure, presumably tetragonal I4/mcm with tilted oxygen octahedra as it has been observed in EuTiO3. The magnetic measurements show that the antiferromagnetic order occurs below 1.8 K. Eu0.5Ba0.25Sr0.25TiO3 has three times lower coercive field than Eu0.5Ba0.5TiO3, therefore we propose this system for measurements of electric dipole moment of electron.
The structural phase transition in hexagonal BaMnO$_3$ occurring at $T_c$=130 K was studied in ceramic samples using electron and X-ray diffraction, second harmonic generation as well as by dielectric and lattice dynamic spectroscopies. The low-temperature phase (space group $P6_{3}cm$) is ferroelectric with a triplicated unit cell. The phase transition is driven by an optical soft mode from the Brillouin-zone boundary [$q = (frac{1}{3},frac{1}{3},0)$]; this mode activates in infrared and Raman spectra below $T_c$ and it hardens according to the Cochran law. Upon cooling below $T_c$, the permittivity exhibits an unusual linear increase with temperature; below 60 K, in turn, a frequency-dependent decrease is observed, which can be explained by slowing-down of ferroelectric domain wall motions. Based on our data we could not distinguish whether the high-temperature phase is paraelectric or polar (space groups $P6_{3}/mmc$ or $P6_{3}mc$, respectively). Both variants of the phase transition to the ferroelectric phase are discussed based on the Landau theory. Electron paramagnetic resonance and magnetic susceptibility measurements reveal an onset of one-dimensional antiferromagnetic ordering below $approx220,rm K$ which develops fully near 140 K and, below $T_{n} approx 59,rm K$, it transforms into a three-dimensional antiferromagnetic order.
The coupling between ferroelectric and magnetic orders in multiferroic materials and the nature of magnetoelectric (ME) effects are enduring experimental challenges. In this work, we have studied the response of magnetization to ferroelectric switching in thin-film hexagonal YbFeO3, a prototypical improper multiferroic. The bulk ME decoupling and potential domain-wall ME coupling were revealed using x-ray magnetic circular dichroism (XMCD) measurements with in-situ ferroelectric polarization switching. Our Landau theory analysis suggests that the bulk ME-coupled ferroelectric switching path has a higher energy barrier than that of the ME-decoupled path; this extra barrier energy is also too high to be reduced by the magneto-static energy in the process of breaking single magnetic domains into multi-domains. In addition, the reduction of magnetization around the ferroelectric domain walls predicted by the Landau theory may induce the domain-wall ME coupling in which the magnetization is correlated with the density of ferroelectric domain walls. These results provide important experimental evidence and theoretical insights into the rich possibilities of ME couplings in hexagonal ferrites, such as manipulating the magnetic states by an electric field.