Large magnetocapacitance in electronic ferroelectric manganite systems

We have observed a sizable positive magnetocapacitance ($\sim$$5-90\%$) in perovskite Pr$_{0.55}$Ca$_{0.45}$MnO$_3$ and bilayer Pr(Sr$_{0.1}$Ca$_{0.9}$)$_2$Mn$_2$O$_7$ system under 5T magnetic field across 20-100 K below the magnetic transition point T$_N$. The magnetodielectric effect, on the other hand, exhibits a crossover: (a) from positive to negative for the perovskite system and (b) from negative to positive for the bilayer system over the same temperature range. The bilayer Pr(Sr$_{0.1}$Ca$_{0.9}$)$_2$Mn$_2$O$_7$ system exhibits a sizable anisotropy as well. We have also noticed the influence of magnetic field on the dielectric relaxation characteristics of these systems. These systems belong to a class of improper ferroelectrics and are expected to exhibit charge/orbital order driven ferroelectric polarization below the transition point T$_{CO}$. Large magnetocapacitance in these systems shows typical multiferroic behavior even though the ferroelectric polarization is small in comparison to that of other ferroelectrics.Comment: 6 pages with 5 embedded figures; accepted for publication in J. Appl. Phy

Confined spin waves reveal an assembly of nanosize domains in ferromagnetic La(1-x)CaxMnO3 (x=0.17,0.2)

We report a study of spin-waves in ferromagnetic La$_{1-x}$Ca$_{x}$MnO$_3$, at concentrations x=0.17 and x=0.2 very close to the metallic transition (x=0.225). Below T$_C$, in the quasi-metallic state (T=150K), nearly q-independent energy levels are observed. They are characteristic of standing spin waves confined into finite-size ferromagnetic domains, defined in {\bf a, b) plane for x=0.17 and in all q-directions for x=0.2. They allow an estimation of the domain size, a few lattice spacings, and of the magnetic coupling constants inside the domains. These constants, anisotropic, are typical of an orbital-ordered state, allowing to characterize the domains as "hole-poor". The precursor state of the CMR metallic phase appears, therefore, as an assembly of small orbital-ordered domains.Comment: 4 pages, 5 figure

Spin dynamics of strongly-doped La_{1-x}Sr_xMnO_3

Cold neutron triple-axis measurements have been used to investigate the nature of the long-wavelength spin dynamics in strongly-doped La$_{1-x}$Sr$_{x}$MnO$_3$ single crystals with $x$=0.2 and 0.3. Both systems behave like isotropic ferromagnets at low T, with a gapless ($E_0 < 0.02$ meV) quadratic dispersion relation $E = E_0 + Dq^2$. The values of the spin-wave stiffness constant $D$ are large ($D_{T=0}$ = 166.77 meV$\AA^2$ for $x$=0.2 and D$_{T=0}$ = 175.87 meV$\AA^2$ for $x$=0.3), which directly shows that the electron transfer energy for the $d$ band is large. $D$ exhibits a power law behavior as a function of temperature, and appears to collapse as T -> T_C. Nevertheless, an anomalously strong quasielastic central component develops and dominates the fluctuation spectrum as T -> T_C. Bragg scattering indicates that the magnetization near $T_C$ exhibits power law behavior, with $\beta \simeq 0.30$ for both systems, as expected for a three-dimensional ferromagnet.Comment: 4 pages (RevTex), 3 figures (encapsulated postscript

Electric field driven destabilization of the insulating state in nominally pure LaMnO3

We report an electric field driven destabilization of the insulating state in nominally pure LaMnO3 single crystal with a moderate field which leads to a resistive state transition below 300 K. The transition is between the insulating state in LaMnO3 and a high resistance bad metallic state that has a temperature independent resistivity. The transition occurs at a threshold field (Eth) which shows a steep enhancement on cooling. While at lower temperatures the transition is sharp and involves large change in resistance but it softens on heating and eventually absent above 280K. When the Mn4+ content is increased by Sr substitution up to x=0.1, the observed transition though observable in certain temperature range, softens considerably. The observation has been explained as bias driven percolation type transition between two coexisting phases, where the majority phase is a charge and orbitally ordered polaronic insulating phase and the minority phase is a bad metallic phase. The mobile fraction f of the bad metallic phase deduced from the experimental data follows an activated kinetics with the activation energy nearly equal to 200 meV and the prefactor fo is a strong function of the field that leads to a rapid enhancement of f on application of field leading to the resistive state transition. We suggest likely scenarios for such co-existing phases in nominally pure LaMnO3 that can lead to the bias driven percolation type transition.Comment: Accepted in JPC

Nonequilibrium 1/f Noise in Low-doped Manganite Single Crystals

1/f noise in current biased La0.82Ca0.18MnO3 crystals has been investigated. The temperature dependence of the noise follows the resistivity changes with temperature suggesting that resistivity fluctuations constitute a fixed fraction of the total resistivity, independently of the dissipation mechanism and magnetic state of the system. The noise scales as a square of the current as expected for equilibrium resistivity fluctuations. However, at 77 K at bias exceeding some threshold, the noise intensity starts to decrease with increasing bias. The appearance of nonequilibrium noise is interpreted in terms of bias dependent multi-step indirect tunneling.Comment: 4pages, 3figures,APL accepte

Magnetic and Optical properties of strained films of multiferroic GdMnO3

The effects of strain on a film of mulitferroic GdMnO3 are investigated using both magnetometry and magneto-optic spectroscopy. Optical spectra, in the energy range 1.5eV - 3.5eV, were taken in Faraday geometry in an applied magnetic field and also at remanence. This yielded rich information on the effects of strain on the spin ordering in these films. Epitaxial films of GdMnO3 were grown on SrTiO3 and LaAlO3 substrates. The LaAlO3 was twinned and so produced a highly strained film whereas the strain was less for the film grown on SrTiO3. The Ne\'el temperatures and coercive fields were measured using zero field data and hysteresis loops obtained using a SQUID magnetometer. Optical absorption data agreed with earlier work on bulk materials. The two well known features in the optical spectrum, the charge transfer transition between Mn d states at ~2eV and the band edge transition from the oxygen p band to the d states at ~3eV are observed in the magnetic circular dichroism; however they behaved very differently both as a function of magnetic field and temperature. This is interpreted in terms of the magnetic ordering of the Mn spins.Comment: 9 pages of text including figure

Ferromagnetic domain structure of La0.78Ca0.22MnO3 single crystals

The magneto-optical technique has been employed to observe spontaneous ferromagnetic domain structures in La0.78Ca0.22MnO3 single crystals. The magnetic domain topology was found to be correlated with the intrinsic twin structure of the investigated crystals. With decreasing temperature the regular network of ferromagnetic domains undergoes significant changes resulting in apparent rotation of the domain walls in the temperature range of 70–150 K. The apparent rotation of the domain walls can be understood in terms of the Jahn-Teller deformation of the orthorhombic unit cell, accompanied by additional twinning