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Register a new userAbsence of ferroelectricity in BiMnO3 ceramics
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We performed factor-group analysis of all phonons in possible monoclinic C2/c and C2 structures of BiMnO3 and compared it with our experimental infrared and Raman spectra. We conclude that the crystal structure is centrosymmetric C2/c in the whole investigated temperature range from 10 to 550 K, therefore BiMnO3 cannot be ferroelectric. We revealed a dielectric relaxation in THz spectra above the structural phase transition taking place at T_C1=475 K giving evidence in strong lattice anharmonicity and a large dynamical disorder of Bi cations above T_C1. Step-like dielectric anomaly observed at T_C1 in THz permittivity reminds antiferroelectric phase transition. Nevertheless, the low-temperature dielectric studies did not reveal any antiferroelectric or ferroelectric hysteresis loop. Our experimental results support theoretical paper of P. Baettig et al. (J. Am. Chem. Soc. 129, 9854 (2007)) claiming that BiMnO3 is not multiferroic, but only antipolar ferromagnet.
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We studied the ferroelectric and ferromagnetic properties of compressive strained and unstrained BiMnO3 thin films grown by rf-magnetron sputtering. BiMnO3 samples exhibit a 2D cube-on-cube growth mode and a pseudo-cubic struc-ture up to a thickness of 15 nm and of 25 nm when deposited on (001) SrTiO3 and (110) DyScO3, respectively. Above these thicknesses we observe a switching to a 3D island growth and a simultaneous structural change to a monoclinic structure characterized by a (00l) orientation of the monoclinic unit cell. While ferromagnetism is observed below Tc = 100 K for all samples, signatures of room temperature ferroelectricity were found only in the pseudo-cubic ultra-thin films, indicating a correlation between electronic and structural orders.
We present the microscopic theory of improper multiferroicity in BiMnO3, which can be summarized as follows: (1) the ferroelectric polarization is driven by the hidden antiferromagnetic order in the otherwise centrosymmetric C2/c structure; (2) the relativistic spin-orbit interaction is responsible for the canted spin ferromagnetism. Our analysis is supported by numerical calculations of electronic polarization using Berrys phase formalism, which was applied to the low-energy model of BiMnO3 derived from the first-principles calculations. We explicitly show how the electric polarization can be controlled by the magnetic field and argue that BiMnO3 is a rare and potentially interesting material where ferroelectricity can indeed coexist and interplay with the ferromagnetism.
Electromagnons are known from multiferroics as spin waves excited by the electric component of electromagnetic radiation. We report the discovery of an excitation in the far-infrared spectra of eps-Fe2O3 which we attribute to an electromagnon appearing below 110 K, where the ferrimagnetic structure becomes incommensurately modulated. Inelastic neutron scattering shows that the electromagnon energy corresponds to that of a magnon from the Brillouin zone boundary. Dielectric measurements did not reveal any sign of ferroelectricity in eps-Fe2O3 down to 10 K, despite its acentric crystal structure. This shows that the activation of an electromagnon requires, in addition to the polar ferrimagnetic structure, a modulation of the magnetic structure. We demonstrate that a combination of inelastic neutron scattering with infrared and / or terahertz spectroscopies allows detecting electromagnons in ceramics, where no crystal-orientation analysis of THz and infrared spectra is possible.
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.
Single crystal synthesis, structure, electric polarization and heat capacity measurements on hexagonal InMnO3 show that this small R ion in the RMnO3 series is ferroelectric (space group P63cm). Structural analysis of this system reveals a high degree of order within the MnO5 polyhedra but significant distortions in the R-O bond distributions compared to the previously studied materials. Point-charge estimates of the electric polarization yield an electrical polarization of approximately 7.8 micro C/cm^2, 26% larger than the well-studied YMnO3 system. This system with enhanced room temperature polarization values may serve as a possible replacement for YMnO3 in device application.
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