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

Dielectric anomaly at the orbital order-disorder transition in LaMnO3+δ

We report a novel dielectric anomaly around the Jahn-Teller orbital orderdisorder transition temperature TJT in LaMnO3+δ. The transition has been characterized by resistivity (ρ) vs. temperature (T), calorimetry, and temperature dependent X-ray diffraction studies. Measurements of complex dielectric permittivity ε* (= ε'+ iε") over a low frequency range (1 Hz -10 MHz) across TJT reveal distinct anomaly. This observation and the reported relatively high static dielectric constant at T = 0 (ε0 ~ 18-20), possibly, indicate that the orbital order gives rise to intrinsic polarization that undergoes transition at TJT. The frequency dispersion of the dielectric response at any given temperature, however, reveals that the dielectric response consists of Maxwell-Wagner component, due to interfaces, within such low frequency range. The TJT and the nature of the anomaly in ε'(ω,T), ε"(ω,T) at TJT, of course, vary - from sharp upward feature to a smeared plateau and then a downward trend - depending on the Mn4+ concentration of the sample. The observation of intrinsic dielectric response due to long-range orbital order in LaMnO3 - where no ferroelectric order is possible due to the absence of offcenter distortion in MnO6 octahedra - may throw a new light on these classes of materials vis-à-vis multiferroic materials

Current-driven orbital order-disorder transition in LaMnO3

We report significant influence of electric current on the orbital order-disorder transition in LaMnO3. The transition temperature T_OO, thermal hysteresis in the resistivity (rho) versus temperature (T) plot around T_OO, and latent heat L associated with the transition decrease with the increase in current density. Eventually, at a critical current density, L reaches zero. The transition zone, on the other hand, broadens with the increase in current density. The states at ordered, disordered, and transition zone are all found to be stable within the time window from ~10^-3 to ~10^4 seconds.Comment: 7 pages including 5 figures; resolution of Fig.1 is better here than the published versio

Dielectric anomaly at the orbital order-disorder transition in LaMnO_(3+delta)

We report a novel dielectric anomaly around the Jahn-Teller orbital order-disorder transition temperature T_JT in LaMnO_(3+delta). The transition has been characterized by resistivity (rho)versus temperature (T), calorimetry, and temperature-dependent X-ray diffraction studies. Measurements of complex dielectric permittivity epsilon* (= epsilon'-i.epsilon'') over a low-frequency range (1 Hz - 10 MHz)across T_JT reveal a distinct anomaly. This observation, and the reported relatively high static dielectric constant at T = 0 (epsilon0 \~18-20), possibly indicate that the orbital order gives rise to intrinsic polarization that undergoes transition at T_JT. The frequency dispersion of the dielectric response at any given temperature, however, reveals that the dielectric response consists of Maxwell-Wagner component, due to interfaces, within such a low frequency range. The T_JT and the nature of the anomaly in epsilon'(omega,T), epsilon''(omega,T) at T_JT, of course, vary - from a sharp upward feature to a smeared plateau and then a downward trend - depending on the Mn^4+ concentration of the sample. The observation of an intrinsic dielectric response due to long-range orbital order in LaMnO_3 - where no ferroelectric order is possible due to the absence of off-centre distortion in MnO_6 octahedra - may throw a new light onto these classes of materials vis-a-vis multiferroic materials.Comment: 22 pages including 7 figures; pdf only; accepted for publication in J.Phys.:Condens. Matte

Evolution of orbital phases with particle size in nanoscale stoichiometric LaMnO3

The thermodynamically stable long-range orbital order in bulk LaMnO3 becomes metastable at nanoscale around a critical particle size d_C~20 nm. The orbital order-disorder transition switches from reversible to irreversible at d_C while the resistance in the orbital ordered state decays by 2-4% over a time scale of ~3000s. At well below d_C, of course, a stable orbital disordered phase emerges. The orthorhombic distortion of the underlying crystallographic structure (space group Pbnm) decreases systematically with the decrease in particle size and at far below d_C (e.g., at ~10 nm), the structure becomes cubic (space group Pm-3m). Using the crystallographic and electrical resistance data, a phase diagram has been constructed showing the evolution of different orbital phases as a function of particle size across ~10 nm to bulk for stoichiometric LaMnO3.Comment: revised following referees' comments, accepted for publicaton in J. Appl. Phy

Dielectric anomaly at T_N in LaMnO3

We observe a distinct anomaly in dielectric permittivity (epsilon') as well as relaxation time (tao_0) versus temperature (T) pattern at the antiferromagnetic transition point (T_N) in single crystal of LaMnO3. The equivalent circuit analysis of the impedance spectra across T_N reveals clear anomaly in the capacitive component C_0 at T_N. Since no structural transition takes place across T_N, the anomaly in tao_0 and C_0 at T_N possibly signifies multiferroicity stemming from coupling between orbital and spin order in LaMnO3.Comment: 14 pages including 3 figures; pdf only; accepted for publication in Phys. Rev.

Particle-size dependence of orbital order-disorder transition in LaMnO3

The latent heat (L) associated with the orbital order-disorder transition at T_JT is found to depend significantly on the average particle size (d) of LaMnO3. It rises slowly with the decrease in d down to ~100 nm and then jumps by more than an order of magnitude in between d ~ 100 nm and ~30 nm. Finally, L falls sharply to zero at a critical particle size d_c ~ 19 nm. The transition temperature T_JT also exhibits an almost similar trend of variation with the particle size, near d ~ 30 nm and below, even though the extent of variation is relatively small. The zero-field-cooled (ZFC) and field-cooled (FC) magnetization versus temperature study over a temperature range 10-300 K reveals that the antiferromagnetic transition temperature decreases with d while the temperature range, over which the ZFC and FC data diverge, increases with the drop in d. The FC magnetization also is found to increase sharply with the drop in particle size. A conjecture of nonmonotonic variation in orbital domain structure with decrease in particle size - from smaller domains with large number of boundaries to larger domains with small number of boundaries due to lesser lattice defects and, finally, down to even finer domain structures with higher degree of metastability - along with increase in surface area in core-shell structure, could possibly rationalize the observed L versus d and T_JT versus d patterns. Transmission electron microscopy data provide evidence for presence of core-shell structure as well as for increase in lattice defects in finer particles.Comment: 26 pages including 5 figures; pdf only; accepted for publication in Phys. Rev.