Screening for electrically conductive defects in thin functional films using electrochemiluminescence

Multifunctional thin films in energy-related devices often must be electrically insulating where a single nanoscale defect can result in complete device-scale failure. Locating and characterizing such defects presents a fundamental problem where high-resolution imaging methods are needed to find defects, but imaging with high spatial resolution limits the field of view and thus the measurement throughput. Here, we present a novel high-throughput method for detecting sub-micron defects in insulating thin films by leveraging the electrochemiluminescence (ECL) of luminol. Through a systematic study of reagent concentrations, buffers, voltage, and excitation time, we identify optimized conditions under which it is possible to detect sub-micron defects at high-throughput. Extrapolating from the signal to background observed for detecting 440 nm wide lines and 620 nm diameter circles, we estimate the minimum detectable features to be lines as narrow as 2.5 nm in width and pinholes as small as 70 nm in radius. We further explore this method by using it to characterize a nominally insulating poly(phenylene oxide) film and find conductive defects that are cross-correlated with high-resolution atomic force microscopy to provide feedback to synthesis. Given this assay's inherent parallelizability and scalability, it is expected to have a major impact on the automated discovery of multifunctional films.