Process temperature-dependent interface quality and Maxwell–Wagner interfacial polarization in atomic layer deposited Al2O3/TiO2 nanolaminates for energy storage applications

Considering the excellent tunability of electrical and dielectric properties in binary metal oxide based multi-layered nanolaminate structures, a thermal atomic layer deposition system is carefully optimized for the synthesis of device grade Al2O3/TiO2 nanolaminates with well-defined artificial periodicity and distinct interfaces, and the role of process temperature in the structural, interfacial, dielectric and electrical properties is systematically investigated. A marginal increase in interfacial interdiffusion in these nanolaminates, at elevated temperatures, is validated using X-ray reflectivity and secondary ion mass spectrometry studies. With an increase in deposition temperature from 150 to 300 °C, the impedance spectroscopy measurements of these nanolaminates exhibited a monotonic increment in dielectric constant from ∼95 to 186, and a decrement in dielectric loss from ∼0.48 to 0.21, while the current-voltage measurements revealed a subsequent reduction in leakage current density from ∼2.24 × 10-5 to 3.45 × 10-7 A cm-2 at 1 V applied bias and an improvement in nanobattery polarization voltage from 100 mV to 700 mV, respectively. This improvement in dielectric and electrical properties at elevated processing temperature is attributed to the reduction in impurity content along with the significant enhancement in sublayer densities and the conductivity contrast driven Maxwell-Wagner interfacial polarisation. Additionally, the devices fabricated at 300 °C exhibited a higher capacitance density of ∼22.87 fF μm-2, a low equivalent oxide thickness of ∼1.51 nm, and a low leakage current density of ∼10-7 A cm-2 (at 1 V bias), making this nanolaminate a promising material for high-density energy storage applications. These findings highlight the ALD process temperature assisted growth chemistry of Al2O3/TiO2 nanolaminates for superior dielectric performance and multifaceted applications.