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

TL;DR

This study reports a dielectric anomaly at the orbital order-disorder transition in LaMnO_(3+delta), suggesting intrinsic polarization related to orbital order and its variation with Mn^4+ concentration, with implications for multiferroic materials.

Contribution

It provides the first evidence of intrinsic dielectric response linked to orbital order in LaMnO_3 without ferroelectric distortion, highlighting a new aspect of orbital physics.

Findings

Dielectric anomaly observed at T_JT in LaMnO_(3+delta)

Intrinsic polarization possibly associated with orbital order

Dielectric response influenced by Mn^4+ concentration

Abstract

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.