Evolution of High Dielectric Permittivity in Low-Temperature Solution Combustion-Processed Phase-Pure High Entropy Oxide (CoMnNiFeCr)O for Thin Film Transistors

Abstract

An investigation of dielectric permittivity on the sintered high entropy oxide (HEO) capacitor composed of Co, Cr, Fe, Mn, and Ni (i.e., (CoCrFeMnNi)O) developed using solution combustion synthesis is performed. Stabilization of the phase in HEO is extremely important as it has a direct influence on the properties. In order to explore phase stabilization, in-depth studies of thermal, structural, morphological, and compositional analyses are carried out. The optimized processing parameters are further implemented on depositing (CoCrFeMnNi)O dielectric thin films followed by a thin film transistor. Irrespective of the reaction medium, the precursors undergo combustion at a low temperature below 250 °C, resulting in amorphous HEO. Upon crystallization at 500 °C, no secondary impurity oxides were detected and phase-stabilized to a spinel structure (Fd3m). A homogeneous distribution of all five cations without any segregation and a completely disordered occupancy of the cations were displayed by the bulk and thin films of HEOs. The spinel (CoCrFeMnNi)O exhibited high permittivity, with values approximately 7.3 × 102(in bulk) and 3 × 101(in a thin film), measured at 1 kHz owing to the entropy stabilization effect of HEO. Due to their high permittivity and low leakage current density (∼10-8A/cm2), the (CoMnNiFeCr)O thin film was integrated into thin film transistors (TFTs) with molybdenum disulfide-channel. TFTs showed a field effect mobility of 8.8 cm2V-1s-1, an on-off ratio of approximately 105, a threshold voltage of -1.5 V, and a subthreshold swing of 0.38 V/dec. The low voltage operation (<5 V) of these TFTs makes solution combustion-derived HEO (CoMnNiFeCr)O a potential candidate in microelectronics and optoelectronics applications. © 2023 ACS Applied Electronic Materials. All rights reserved.