Tunable ion energy barrier modulation through aliovalent halide doping for reliable and dynamic memristive neuromorphic systems.

Memristive neuromorphic computing has emerged as a promising computing paradigm for the upcoming artificial intelligence era, offering low power consumption and high speed. However, its commercialization remains challenging due to reliability issues from stochastic ion movements. Here, we propose an innovative method to enhance the memristive uniformity and performance through aliovalent halide doping. By introducing fluorine concentration into dynamic TiO2-x memristors, we experimentally demonstrate reduced device variations, improved switching speeds, and enhanced switching windows. Atomistic simulations of amorphous TiO2-x reveal that fluoride ions attract oxygen vacancies, improving the reversible redistribution and uniformity. A number of migration barrier calculations statistically show that fluoride ions also reduce the migration energies of nearby oxygen vacancies, facilitating ionic diffusion and high-speed switching. The detailed Voronoi volume analysis further suggests design principles in terms of the migrating species' electrostatic repulsion and migration barriers. This work presents an innovative methodology for the fabrication of reliable memristor devices, contributing to the realization of hardware-based neuromorphic systems.