Small polaron hopping and tunneling transport in Maxwell-Wagner relaxation dominated Al2O3/TiO2 subnanometric laminates

Abstract

Maxwell-Wagner relaxation dominated Al2O3/TiO2 nanolaminates (ATA NLs) have recently demonstrated their potential for high-density energy storage applications. In this report, we have unraveled the defect-mediated transport mechanisms prevailing in Al2O3/TiO2 sub-nanometric laminates. Temperature-dependent ac conductivity measurements revealed the signature of small polaron hopping in TiO2 active layers and trap-assisted tunneling transport through Al2O3 barrier layers, which was corroborated by resonant photoelectron spectroscopy and temperature-dependent current-voltage measurement. The polaronic defect states, found ∼1 eV below the Fermi level, served as the hopping centers and leakage paths for current. The signature of quantum tunneling transport and the negative differential conductance observed toward higher electric field was attributed to the splitting of delocalized minibands. These transport properties of Al2O3/TiO2 nanolaminates will help in tailoring these materials for next-generation storage capacitors.