PhD Final Defense: Harley Quinn

MSE PhD Final Defense: Harley Quinn

TITLE: Development and Implementation of the Polymer Analysis and Discovery Array (PANDA) Platform

ADVISOR: Keith Brown ME, MSE, Physics

COMMITTEE: Abigail Plummer ME, MSE; Andre Sharon MSE, ME; Jörg Werner ME, MSE, Chemistry; Chair:

ABSTRACT: Multifunctional thin films are ubiquitous in modern technology, yet designing such films with multiple distinct functionalities remains tedious and manual. This thesis explores approaches to accelerate the discovery and optimization of such films through the development of novel assays and hardware platforms that provide new actionable information while addressing key bottlenecks from manual materials optimization. First, we develop a high-throughput electrochemiluminescence (ECL) method for detecting sub-micron conductive defects in insulating thin films. By tuning reagent concentrations, buffers conditions, applied voltage, and excitation time, we maximize the luminol ECL signal, enabling detection of sub-micron defects to the point that crack features as small as 2.5 nm in width are in principle detectable. This non-destructive approach supports automated, scalable characterization across large areas to enable the development of electrically insulating films for applications including solid-state battery electrolytes. We then develop and validate a self-driving lab (SDL), namely the polymer analysis and discovery array (PANDA), that can perform both the synthesis and characterization of functional polymer films without human intervention. This involved an iterative design process followed by extensive validation experiments to confidently use the custom fluid handling, optical analysis, and electrochemical modules. As a proof-of-concept, we used the PANDA to autonomously optimize the electrochromic switching of electrodeposited poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) films. Finally, we customize and improve the PANDA for applications in surface science to realize PANDA-film. Specifically, we extended the PANDA platform to incorporate automated vial capping/decapping, higher precision and speed fluid handling, and controlled illumination to perform automated wetting measurements of electrodeposited films. Together, these advances provide a generalizable path to rapid, closed-loop optimization of multifunctional thin films by coupling high-throughput assays, autonomous experimentation, and learning-guided decision making. Going forward, these modular platforms and assays can be rapidly applied to identify high performing multi-functional polymer films.