We have studied the crystal and magnetic structures of the magnetoelectric materials RMn 2 O 5 ͑R =Tb,Ho,Dy͒ using neutron diffraction as a function of temperature. All three materials display incommensurate antiferromagnetic ordering below 40 K, becoming commensurate on further cooling. For R =Tb,Ho, a commensurate-incommensurate transition takes place at low temperatures. The commensurate magnetic structures have been solved and are discussed in terms of competing exchange interactions. The spin configuration within the ab plane is essentially the same for each system, and the radius of R determines the sign of the magnetic exchange between adjacent planes. The inherent magnetic frustration in these materials is lifted by a small lattice distortion, primarily involving shifts of the Mn 3+ cations and giving rise to a canted antiferroelectric phase.

We have investigated the detailed magnetic field dependence of the electric polarization and dielectric constant in (Tb,Dy,Ho)Mn2O5 where magnetic and ferroelectric transitions are intimately coupled. Our fundamental discovery is the unprecedented large change of the dielectric constant with magnetic field, particularly in DyMn2O5, associated with an unusual commensurate-incommensurate magnetic transition. This extraordinary effect appears to originate from the high sensitivity of the incommensurate state to external perturbation.

Spin glasses are founded in the frustration and randomness of microscopic magnetic interactions. They are non-ergodic systems where replica symmetry is broken. Although magnetic glassy behaviour has been observed in many colossal magnetoresistive manganites, there is no consensus that they are spin glasses. Here, an intriguing glass transition in (La,Pr,Ca)MnO3 is imaged using a variable-temperature magnetic force microscope. In contrast to the speculated spin-glass picture, our results show that the observed static magnetic configuration seen below the glass-transition temperature arises from the cooperative freezing of the first-order antiferromagnetic (charge ordered) to ferromagnetic transition. Our data also suggest that accommodation strain is important in the kinetics of the phase transition. This cooperative freezing idea has been applied to structural glasses including window glasses and supercooled liquids, and may be applicable across many systems to any first-order phase transition occurring on a complex free-energy landscape.

We have measured the optical conductivity of single crystal LuMnO3 from 10 to 45000 cm(-1) at temperatures between 4 and 300 K. A symmetry allowed on-site Mn d-d transition near 1.7 eV is observed to blueshift ( approximately 0.1 eV) in the antiferromagnetic state due to Mn-Mn superexchange interactions. Similar anomalies are observed in the temperature dependence of the TO phonon frequencies which arise from spin-phonon interaction. We find that the known anomaly in the temperature dependence of the quasistatic dielectric constant epsilon(0) below T(N) approximately 90 K is overwhelmingly dominated by the phonon contributions.