Maxwell–Wagner Relaxation-Driven High Dielectric Constant in Al2O3/TiO2 Nanolaminates Grown by Pulsed Laser Deposition

Multilayer nanolaminates (NLs) of alternate ultrathin sublayers of Al2O3 and TiO2 (ATA) with the thickness ranging ∼2 to 0.5 nm were fabricated by optimized pulsed laser deposition (PLD). Maxwell-Wagner (M-W) relaxation-induced interfacial polarization was realized and engineered by precisely controlling the sublayer thicknesses and the number of interfaces. X-ray reflectivity and cross-sectional transmission electron microscopy measurements of ATA NLs revealed an artificial periodicity with well-defined uniformly thick amorphous sublayers with chemically and physically distinct interfaces down to a sublayer thickness of ∼0.8 nm. The dielectric constants and loss of ATA NLs were found to increase from ∼60 to 670 and decrease from ∼0.9 to 0.16, respectively, as sublayer thicknesses reduced from ∼2 to 0.8 nm. However, for a sublayer thickness below 0.8 nm, the trend was reversed. Furthermore, temperature-dependent impedance spectroscopy studies revealed two distinct thermally activated relaxation processes, corresponding to TiO2 and Al2O3 sublayers, corroborating the M-W relaxation. The conductivity contrast between the sublayers of ATA NLs enhanced with reducing sublayer thickness and plateaued at a sublayer thickness of ∼0.8 nm, resulting in dominant M-W interfacial polarization and a high cut-off frequency of ∼50 kHz. These results demonstrate that ATA NLs grown by PLD may find application as potential high-k materials for next-generation nanoelectronic devices.