Dynamics of relaxor ferroelectrics

We study a dynamic model of relaxor ferroelectrics based on the spherical random-bond---random-field model and the Langevin equations of motion. The solution to these equations is obtained in the long-time limit where the system reaches an equilibrium state in the presence of random local electric fields. The complex dynamic linear and third-order nonlinear susceptibilities $\chi_1(\omega)$ and $\chi_3(\omega)$, respectively, are calculated as functions of frequency and temperature. In analogy with the static case, the dynamic model predicts a narrow frequency dependent peak in $\chi_3(T,\omega)$, which mimics a transition into a glass-like state.Comment: 15 pages, Revtex plus 5 eps figure

Dynamics of relaxor ferroelectrics

We study a dynamic model of relaxor ferroelectrics based on the spherical random-bond---random-field model and the Langevin equations of motion. The solution to these equations is obtained in the long-time limit where the system reaches an equilibrium state in the presence of random local electric fields. The complex dynamic linear and third-order nonlinear susceptibilities $\chi_1(\omega)$ and $\chi_3(\omega)$, respectively, are calculated as functions of frequency and temperature. In analogy with the static case, the dynamic model predicts a narrow frequency dependent peak in $\chi_3(T,\omega)$, which mimics a transition into a glass-like state.Comment: 15 pages, Revtex plus 5 eps figure

Materials with Colossal Dielectric Constant: Do They Exist?

Experimental evidence is provided that colossal dielectric constants, epsilon >= 1000, sometimes reported to exist in a broad temperature range, can often be explained by Maxwell-Wagner type contributions of depletion layers at the interface between sample and contacts, or at grain boundaries. We demonstrate this on a variety of different materials. We speculate that the largest intrinsic dielectric constant observed so far in non-ferroelectric materials is of order 100.Comment: 3 figure

Tuning a sign of magnetoelectric coupling in paramagnetic NH2(CH3)2Al1-xCrx(SO4)*6H2O crystals by metal ion substitution

Hybrid organometallic systems offer a wide range of functionalities, including magnetoelectric interactions. However, the ability to design on-demand ME coupling remains challenging despite a variety of host-guest configurations and ME phases coexistence possibilities. Here, we report the effect of metal-ion substitution on the magnetic and electric properties in the paramagnetic ferroelectric DMAAS crystals. Doing so we are able to induce and even tune a sign of the ME interactions in the paramagnetic ferroelectric state. Both studied samples with 6.5% and 20% of Cr become paramagnetic, contrary to the initial diamagnetic compound. Due to the isomorphous substitution with Cr the ferroelectric phase transition temperature increases nonlinearly, with the shift being larger for the sample with Cr content of 6.5%. A magnetic field applied along the polar c axis increases ferroelectricity for this sample and shifts Tc to higher values, while inverse effects are observed for sample containing 20% of Cr. The ME coupling coefficient of 1.7ns/m found for a crystal with 20% of Cr is among the highest reported up to now. The observed sign change of ME coupling coefficient with a small change in Cr content paves the way for ME coupling engineering.Comment: 7 pages, 6 figures. New Organometallic Magnetoelectric and Ferroelectric compoun

Ground State of Relaxor Ferroelectric Pb(Zn1/3Nb2/3)O3Pb(Zn_{1/3}Nb_{2/3})O_3

High energy x-ray diffraction measurements on Pb(Zn$_{1/3}$Nb$_{2/3}$)O$_3$ (PZN) single crystals show that the system does not have a rhombohedral symmetry at room temperature as previously believed. The new phase (X) in the bulk of the crystal gives Bragg peaks similar to that of a nearly cubic lattice with a slight tetragonal distortion. The Bragg profile remains sharp with no evidence of size broadening due to the polar micro crystals (MC). However, in our preliminary studies of the skin, we have found the expected rhombohedral (R) phase as a surface state. On the other hand, studies on an electric-field poled PZN single crystal clearly indicate a rhombohedral phase at room temperature.Comment: 11 pages with 3 figure

Sr2V3O9 and Ba2V3O9: quasi one-dimensional spin-systems with an anomalous low temperature susceptibility

The magnetic behaviour of the low-dimensional Vanadium-oxides Sr2V3O9 and Ba2V3O9 was investigated by means of magnetic susceptibility and specific heat measurements. In both compounds, the results can be very well described by an S=1/2 Heisenberg antiferromagnetic chain with an intrachain exchange of J = 82 K and J = 94 K in Sr2V3O9 and Ba2V3O9, respectively. In Sr2V3O9, antiferromagnetic ordering at T_N = 5.3 K indicate a weak interchain exchange of the order of J_perp ~ 2 K. In contrast, no evidence for magnetic order was found in Ba2V3O9 down to 0.5 K, pointing to an even smaller interchain coupling. In both compounds, we observe a pronounced Curie-like increase of the susceptibility below 30 K, which we tentatively attribute to a staggered field effect induced by the applied magnetic field. Results of LDA calculations support the quasi one-dimensional character and indicate that in Sr2V3O9, the magnetic chain is perpendicular to the structural one with the magnetic exchange being transferred through VO4 tetrahedra.Comment: Submitted to Phy. Rev.

Colossal dielectric constants in transition-metal oxides

Many transition-metal oxides show very large ("colossal") magnitudes of the dielectric constant and thus have immense potential for applications in modern microelectronics and for the development of new capacitance-based energy-storage devices. In the present work, we thoroughly discuss the mechanisms that can lead to colossal values of the dielectric constant, especially emphasising effects generated by external and internal interfaces, including electronic phase separation. In addition, we provide a detailed overview and discussion of the dielectric properties of CaCu3Ti4O12 and related systems, which is today's most investigated material with colossal dielectric constant. Also a variety of further transition-metal oxides with large dielectric constants are treated in detail, among them the system La2-xSrxNiO4 where electronic phase separation may play a role in the generation of a colossal dielectric constant.Comment: 31 pages, 18 figures, submitted to Eur. Phys. J. for publication in the Special Topics volume "Cooperative Phenomena in Solids: Metal-Insulator Transitions and Ordering of Microscopic Degrees of Freedom

Dielectric signature of charge order in lanthanum nickelates

Three charge-ordering lanthanum nickelates La2-xAxNiO4, substituted with specific amounts of A = Sr, Ca, and Ba to achieve commensurate charge order, are investigated using broadband dielectric spectroscopy up to GHz frequencies. The transition temperatures of the samples are characterized by additional specific heat and magnetic susceptibility measurements. We find colossal magnitudes of the dielectric constant for all three compounds and strong relaxation features, which partly are of Maxwell-Wagner type arising from electrode polarization. Quite unexpectedly, the temperature-dependent colossal dielectric constants of these materials exhibit distinct anomalies at the charge-order transitions.Comment: 7 pages, 6 figure

Tuning a sign of magnetoelectric coupling in paramagnetic NH2(CH3)(2)Al1-xCrx(SO4)(2) x 6H(2)O crystals by metal ion substitution

Hybrid organometallic systems offer a wide range of functionalities, including magnetoelectric (ME) interactions. However, the ability to design on-demand ME coupling remains challenging despite a variety of host-guest configurations and ME phases coexistence possibilities. Here, we report the effect of metal-ion substitution on the magnetic and electric properties in the paramagnetic ferroelectric NH2(CH3)(2)Al1-xCrx(SO4)(2) x 6H(2)O. Doing so we are able to induce and even tune a sign of the ME interactions, in the paramagnetic ferroelectric (FE) state. Both studied samples with x = 0.065 and x = 0.2 become paramagnetic, contrary to the initial diamagnetic compound. Due to the isomorphous substitution with Cr the ferroelectric phase transition temperature (T-c) increases nonlinearly, with the shift being larger for the 6.5% of Cr. A magnetic field applied along the polar c axis increases ferroelectricity for the x = 0.065 sample and shifts Tc to higher values, while inverse effects are observed for x = 0.2. The ME coupling coefficient alpha(ME) = 1.7 ns/m found for a crystal with Cr content of x = 0.2 is among the highest reported up to now. The observed sign change of aME with a small change in Cr content paves the way for ME coupling engineering

Dielectric properties and dynamical conductivity of LaTiO3: From dc to optical frequencies

We provide a complete and detailed characterization of the temperature-dependent response to ac electrical fields of LaTiO3, a Mott-Hubbard insulator close to the metal-insulator transition. We present combined dc, broadband dielectric, mm-wave, and infrared spectra of ac conductivity and dielectric constant, covering an overall frequency range of 17 decades. The dc and dielectric measurements reveal information on the semiconducting charge-transport properties of LaTiO3, indicating the importance of Anderson localization, and on the dielectric response due to ionic polarization. In the infrared region, the temperature dependence of the phonon modes gives strong hints for a structural phase transition at the magnetic ordering temperature. In addition, a gap-like electronic excitation following the phonon region is analyzed in detail. We compare the results to the soft-edge behavior of the optical spectra characteristic for Mott-Hubbard insulators. Overall a consistent picture of the charge-transport mechanisms in LaTiO3 emerges.Comment: 11 pages, 8 figures, 1 tabl