Controlling mass transport and topotactic phase transition processes in oxide thin films
EMSL Project ID
60681
Abstract
The overarching goal of this proposal is to understand, predict, and ultimately control mass transport and mass transport induced topotactic phase transition (TPT) processes occurring in structurally ordered transition metal oxide (TMO) thin films and multilayers. The fundamental science we propose is highly relevant to energy/information storage technologies, as such fundamental processes governing the working/failure mechanisms of widely used electrode, electrolyte, and redox-driven resistive switching materials. TPTs occurring at the forefront of redox reactions and electrode/electrolyte interfaces are often responsible for many of the challenges (e.g., safety concern due to volume expansion and capacity decrease after cycling due to loss of desired structure/phase) found in lithium ion batteries and solid oxide fuel cells. Built on the success from past EMSL support (>20 publications in FY18-19, 13 invited talks delivered), we will further investigate structurally and compositionally well-defined complex oxide films and thin-film based devices for the facile intercalation of either lithium cations (Li+ in all-solid-state batteries) or oxygen anions (O2- in memristor devices). Our team will bring together 1) state-of-the-art synthesis of oxide thin film heterostructures and devices; 2) detailed in situ/in operando characterization of the superstructures, film/substrate, film/film, film/vacuum, and film/solvent interfaces, and their evolution as a function of interfacial strain, doping level, and processing conditions; and 3) ab initio modeling of defect formation, structural ordering, and phase transition pathways and kinetics within the studied materials. The specific aims of this research are to: 1) correlate atomic-scale structural evolution, mesoscale topotactic phase transition, and macroscopic mass transport characteristics as TPTs; 2) understand how interfacial epitaxy and interfacial strain can be used to modify the onset (e.g., temperature, electrochemical potential), dynamics, intermediate states, and trajectories of TPTs occurring at solid-solid interfaces.
The unique and powerful synthesis, characterization, and high-performance computing capabilities in EMSL will allow us to establish defensible structure-stability-property relationships. By controlling the onset and trajectories of the TPTs, metastable phases with desired functional properties can be designed, synthesized, stabilized, and harnessed for technological benefits. The fundamental insights gained through this work are of direct relevance to the catalysis, solid oxide fuel cell, information storage and battery research.
Project Details
Start Date
2023-01-04
End Date
2023-10-01
Status
Closed
Released Data Link
Team
Principal Investigator