Interplay between proton ordering and ferroelectric polarization in H-bonded KDP-type crystals

The origin of ferroelectricity in KH_2PO_4 (KDP) is studied by first-principles electronic structure calculations. In the low-temperature phase, the collective off-center ordering of the protons is accompanied by an electronic charge delocalization from the "near" and localization at the "far" oxygen within the O-H...O bonds. Electrostatic forces, then, push the K+ ions towards off-center positions, and induce a macroscopic polarization. The analysis of the correlation between different geometrical and electronic quantities, in connection with experimental data, supports the idea that the role of tunnelling in isotopic effects is irrelevant. Instead, geometrical quantum effects appear to play a central role.Comment: 8 pages, 2 postscript figures, submitted to the X Conference on Computational Materials Science, Villasimius, Sardinia (Italy), 200

Nuclear-spin relaxation of 207^{207}Pb in ferroelectric powders

Motivated by a recent proposal by O. P. Sushkov and co-workers to search for a P,T-violating Schiff moment of the $^{207}$Pb nucleus in a ferroelectric solid, we have carried out a high-field nuclear magnetic resonance study of the longitudinal and transverse spin relaxation of the lead nuclei from room temperature down to 10 K for powder samples of lead titanate (PT), lead zirconium titanate (PZT), and a PT monocrystal. For all powder samples and independently of temperature, transverse relaxation times were found to be $T_2\approx 1.5$ms, while the longitudinal relaxation times exhibited a temperature dependence, with $T_1$ of over an hour at the lowest temperatures, decreasing to $T_1\approx 7$s at room temperature. At high temperatures, the observed behavior is consistent with a two-phonon Raman process, while in the low temperature limit, the relaxation appears to be dominated by a single-phonon (direct) process involving magnetic impurities. This is the first study of temperature-dependent nuclear-spin relaxation in PT and PZT ferroelectrics at such low temperatures. We discuss the implications of the results for the Schiff-moment search.Comment: 6 pages, 4 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

Coexistence of the Critical Slowing Down and Glassy Freezing in Relaxor Ferroelectrics

We have developed a dynamical model for the dielectric response in relaxor ferroelectrics which explicitly takes into account the coexistence of the critical slowing down and glassy freezing. The application of the model to the experiment in PMN allowed for the reconstruction of the nonequilibrium spin glass state order parameter and its comparison with the results of recent NMR experiment (Blinc et al., Phys. Rev. Lett. 83, No. 2 (1999)). It is shown that the degree of the local freezing is rather small even at temperatures where the field-cooled permittivity exceeds the frequency dependent permittivity by an order of magnitude. This observation indicates the significant role of the critical slowing down (accompanying the glass freezing) in the system dynamics. Also the theory predicts an important interrelationship between the frequency dependent permittivity and the zero-field-cooled permittivity, which proved to be consistent with the experiment in PMN (A. Levstik et. al., Phys. Rev. B 57, 11204 (1998))

The polymer phase of the TDAE-C60_{60} organic ferromagnet

The high-pressure Electron Spin Resonance (ESR) measurements were preformed on TDAE-C$_{60}$ single crystals and stability of the polymeric phase was established in the $P - T$ parameter space. At 7 kbar the system undergoes a ferromagnetic to paramagnetic phase transition due to the pressure-induced polymerization. The polymeric phase remains stable after the pressure release. The depolymerization of the pressure-induced phase was observed at the temperature of 520 K. Below room temperature, the polymeric phase behaves as a simple Curie-type insulator with one unpaired electron spin per chemical formula. The TDAE$^+$ donor-related unpaired electron spins, formerly ESR-silent, become active above the temperature of 320 K and the Curie-Weiss behavior is re-established.Comment: Submitted to Phys. Rev.

Phase transitions and quantum effects in anharmonic crystals

The most important recent results in the theory of phase transitions and quantum effects in quantum anharmonic crystals are presented and discussed. In particular, necessary and sufficient conditions for a phase transition to occur at some temperature are given in the form of simple inequalities involving the interaction strength and the parameters describing a single oscillator. The main characteristic feature of the theory is that both mentioned phenomena are described in one and the same setting, in which thermodynamic phases of the model appear as probability measures on path spaces. Then the possibility of a phase transition to occur is related to the existence of multiple phases at the same values of the relevant parameters. Other definitions of phase transitions, based on the non-differentiability of the free energy density and on the appearance of ordering, are also discussed