Electric-field-induced insulator to Coulomb glass transition via oxygen-vacancy migration in Ca-dopedBiFeO3

Abstract

The multiferroic $\mathrm{BiFe}{\mathrm{O}}_{3}$ (BFO) as a charge-transfer-type insulator is an interesting system in which to explore correlated electronic conduction. Here, we substitute divalent Ca ions into the parent BFO and apply an external electric field at elevated temperatures to spatially redistribute spontaneously created oxygen vacancies, thereby generating hole carriers in regions of less dense oxygen-vacancy concentrations. X-ray diffraction and photoemission spectroscopic measurement are employed to quantify a large variation of local oxygen-vacancy concentration, as much as $\ensuremath{\sim}{10}^{21}\phantom{\rule{0.16em}{0ex}}\mathrm{c}{\mathrm{m}}^{\ensuremath{-}3}$, and explore the consequent evolution of electronic band structure. We find that a nonrigid polaronic band is created by hole doping as a result of a strong electron-lattice coupling. We also show strong evidence for the disorder-driven formation of a Coulomb-glass state through electronic transport measurements on a quantitative level. These spectroscopic and transport results can be combined and understood in the framework of intrinsic spatial inhomogeneity of the polaronic charge density. The finding not only offers a promising platform and methodology for examining the interplay of functional defects and correlated electronic behaviors, but also suggests a unique electronic conduction mechanism applicable to systems with coexistence of strong electron correlation, electron-lattice interaction, and randomness beyond the Coulomb-glass physics in semiconductors.