Electronic structure and bond competition in the polar magnet PbVO3_3

Density functional electronic structure studies of tetragonal PbVO$_3$ are reported. The results show a an important role for both Pb 6$p$ - O 2$p$ and V $d$ - O $p$ bonding, with an interplay between these. This is discussed in relation to the possibility of obtaining magnetoelectric behavior.Comment: 5 page

Poling effect on distribution of quenched random fields in a uniaxial relaxor ferroelectric

The frequency dependence of the dielectric permitivity's maximum has been studied for poled and unpoled doped relaxor strontium barium niobate $Sr_{0.61}Ba_{0.39}Nb_{2}O_{6}:Cr^{3+}$ (SBN-61:Cr). In both cases the maximum found is broad and the frequency dispersion is strong. The present view of random fields compensation in the unpoled sample is not suitable for explaining this experimental result. We propose a new mechanism where the dispersion of quenched random electric fields, affecting the nanodomains, is minimized after poling. We test our proposal by numerical simulations on a random field Ising model. Results obtained are in agreement with the polarization's measurements presented by Granzow et al. [Phys. Rev. Lett {\bf 92}, 065701 (2004)].Comment: 7 pages, 4 figure

Magnetic control of large room-temperature polarization

Numerous authors have referred to room-temperature magnetic switching of large electric polarizations as The Holy Grail of magnetoelectricity.We report this long-sought effect using a new physical process of coupling between magnetic and ferroelectric relaxor nano-regions. Here we report magnetic switching between the normal ferroelectric state and the ferroelectric relaxor state. This gives both a new room-temperature, single-phase, multiferroic magnetoelectric, PbZr0.46Ti0.34Fe0.13W0.07O3, with polarization, loss (<4%), and resistivity (typically 108 -109 ohm.cm) equal to or superior to BiFeO3, and also a new and very large magnetoelectric effect: switching not from +Pr to negative Pr with applied H, but from Pr to zero with applied H of less than a Tesla. This switching of the polarization occurs not because of a conventional magnetically induced phase transition, but because of dynamic effects: Increasing H lengthens the relaxation time by x500 from 100 ?s, and it couples strongly the polarization relaxation and spin relaxations. The diverging polarization relaxation time accurately fits a modified Vogel-Fulcher Equation in which the freezing temperature Tf is replaced by a critical freezing field Hf that is 0.92 positive/negative 0.07 Tesla. This field dependence and the critical field Hc are derived analytically from the spherical random bond random field (SRBRF) model with no adjustable parameters and an E2H2 coupling. This device permits 3-state logic (+Pr,0,negative Pr) and a condenser with >5000% magnetic field change in its capacitance.Comment: 20 pages, 5 figure

Tetragonal tungsten bronze compounds: relaxor vs mixed ferroelectric - dipole glass behavior

We demonstrate that recent experimental data (E. Castel et al J.Phys. Cond. Mat. {\bf 21} (2009), 452201) on tungsten bronze compound (TBC) Ba$_2$Pr$_x$Nd$_{1-x}$FeNb$_4$O$_{15}$ can be well explained in our model predicting a crossover from ferroelectric ($x=0$) to orientational (dipole) glass ($x=1$), rather then relaxor, behavior. We show, that since a "classical" perovskite relaxor like Pb(Mn$_{1/3}$ Nb$_{2/3}$)O$_3$ is never a ferroelectric, the presence of ferroelectric hysteresis loops in TBC shows that this substance actually transits from ferroelectric to orientational glass phase with $x$ growth. To describe the above crossover theoretically, we use the simple replica-symmetric solution for disordered Ising model.Comment: 5 two-column pages, 4 figure

Landau Theory of Domain Wall Magnetoelectricity

We calculate the exact analytical solution to the domain wall properties in a multiferroic system with two order parameters that are coupled bi-quadratically. This is then adapted to the case of a magnetoelectric multiferroic material such as BiFeO3, with a view to examine critically whether the domain walls can account for the enhancement of magnetization reported for thin films fo this material, in view of the correlation between increasing magnetization and increasing volume fraction of domain walls as films become thinner. The present analysis can be generalized to describe a class of magnetoelectric devices based upon domain walls rather than bulk properties.Comment: 9 pages, 4 figure

Raman and Infrared-Active Phonons in Hexagonal HoMnO3_3 Single Crystals: Magnetic Ordering Effects

Polarized Raman scattering and infrared reflection spectra of hexagonal HoMnO$_3$ single crystals in the temperature range 10-300 K are reported. Group-theoretical analysis is performed and scattering selection rules for the second order scattering processes are presented. Based on the results of lattice dynamics calculations, performed within the shell model, the observed lines in the spectra are assigned to definite lattice vibrations. The magnetic ordering of Mn ions, which occurs below T$_N$=76 K, is shown to effect both Raman- and infrared-active phonons, which modulate Mn-O-Mn bonds and, consequently, Mn exchange interaction.Comment: 8 pages, 6 figure

Polarization Relaxation Induced by Depolarization Field in Ultrathin Ferroelectric BaTiO3_3 Capacitors

Time-dependent polarization relaxation behaviors induced by a depolarization field $E_{d}$ were investigated on high-quality ultrathin SrRuO$_{3}$/BaTiO$_{3}$/SrRuO$_{3}$ capacitors. The $E_d$ values were determined experimentally from an applied external field to stop the net polarization relaxation. These values agree with those from the electrostatic calculations, demonstrating that a large $E_{d}$ inside the ultrathin ferroelectric layer could cause severe polarization relaxation. For numerous ferroelectric devices of capacitor configuration, this effect will set a stricter size limit than the critical thickness issue

Giant Magnetoelectric Effect in a Multiferroic Material with a High Ferroelectric Transition Temperature

We present a unique example of giant magnetoelectric effect in a conventional multiferroic HoMnO3, where polarization is very large (~56 mC/m2) and the ferroelectric transition temperature is higher than the magnetic ordering temperature by an order. We attribute the uniqueness of the giant magnetoelectric effect to the ferroelectricity induced entirely by the off-center displacement of rare earth ions with large magnetic moments. This finding suggests a new avenue to design multiferroics with large polarization and higher ferroelectric transition temperature as well as large magnetoelectric effects

On the phase identity and its thermal evolution of lead free (Bi1/2Na1/2)TiO3-6 mol% BaTiO3

Temperature-dependent dielectric permittivity of 0.94(Bi1/2Na1/2) TiO3-0.06BaTiO(3) (BNT-6BT) lead-free piezoceramics was studied to disentangle the existing unclear issues over the crystallographic aspects and phase stability of the system. Application of existing phenomenological relaxor models enabled the relaxor contribution to the entire dielectric permittivity spectra to be deconvoluted. The deconvoluted data in comparison with the temperature-dependent dielectric permittivity of a classical perovskite relaxor, La-modified lead zirconate titanate, clearly suggest that BNT-6BT belongs to the same relaxor category, which was also confirmed by a comparative study on the temperature-dependent polarization hysteresis loops of both materials. Based on these results, we propose that the low-temperature dielectric anomaly does not involve any phase transition such as ferroelectric-toantiferroelectric. Supported by transmission electron microscopy and X-ray diffraction experiments at ambient temperature, we propose that the commonly observed two dielectric anomalies are attributed to thermal evolution of ferroelectric polar nanoregions of R3c and P4bm symmetry, which coexist nearly throughout the entire temperature range and reversibly transform into each other with temperature.open1128

State transition and electrocaloric effect of BaZrx_{x}Ti1−x_{1-x}O3_3: simulation and experiment

The electrocaloric effect (ECE) of BaZr$_{x}$Ti$_{1-x}$O$_3$ (BZT) is closely related to the relaxor state transition of the materials. This work presents a systematic study on the ECE and the state transition of the BZT, using a combined canonical and microcanonical Monte Carlo simulations based a lattice-based on a Ginzburg-Landau-type Hamiltonian. For comparison and verification, experimental measurements have been carried on BTO and BZT ($x=0.12$ and $0.2$) samples, including the ECE at various temperatures, domain patterns by Piezoresponse Force Microscopy at room temperature, and the P-E loops at various temperatures. Results show that the dependency of BZT behavior of the Zr-concentration can be classified into three different stages. In the composition range of $0 \leq x \leq 0.2$, ferroelectric domains are visible, but ECE peak drops with increasing Zr-concentration harshly. In the range of $0.3 \leq x \leq 0.7$, relaxor features become prominent, and the decrease of ECE with Zr-concentration is moderate. In the high concentration range of $x \geq 0.8$, the material is almost nonpolar, and there is no ECE peak visible. Results suggest that BZT with certain low range of Zr-concentration around $x=0.12 \sim 0.3$ can be a good candidate with relatively high ECE and simutaneously wide temperature application range at rather low temperature