Curating and analyzing centralized data repositories is a valuable approach in resolving the issue of reproducibility, gaining new insights and guiding future experiments, especially in the field of nanomaterials research. In this work, a data set containing processing information and mobility values of 115 DPP-DTT-based organic field effect transistors (OFET) was constructed from 15 publications. A customized classification algorithm was applied to the data set to help identify a reduced design region for polymer solution concentration that would be more likely to result in improved hole mobility. Experiments performed to confirm the insights from the data curation exercise revealed a strong influence of solution concentration on the polymer chain excitonic interactions and electronic performance. Devices fabricated at the critical chain overlap concentration of 5 g/L in chlorobenzene resulted in improved hole mobility, and were in good agreement with the insights provided by the classification algorithm.

The advent of data analytics techniques and materials informatics provides opportunities to accelerate the discovery and development of organic semiconductors for electronic devices. However, the development of engineering solutions is limited by the ability to control thin-film morphology in an immense parameter space. The combination of highthroughput experimentation (HTE) laboratory techniques and data analytics offers tremendous avenues to traverse the expansive domains of tunable variables offered by organic semiconductor thin films. This Perspective outlines the steps required to incorporate a comprehensive informatics methodology into the experimental development of polymer-based organic semiconductor technologies. The translation of solution processing and property metrics to thin-film behavior is crucial to inform efficient HTE for data collection and application of data-centric tools to construct new process−structure−property relationships. We argue that detailed investigation of the solution state prior to deposition in conjunction with thin-film characterization will yield a deeper understanding of the physicochemical mechanisms influencing performance in π-conjugated polymer electronics, with data-driven approaches offering predictive capabilities previously unattainable via traditional experimental means.

No abstract

We explore the application of excitation correlation spectroscopy to detect nonlinear photophysical dynamics in two distinct semiconductor classes through time-integrated photoluminescence and photocurrent measurements. In this experiment, two variably delayed femtosecond pulses excite the semiconductor, and the time-integrated photoluminescence or photocurrent component arising from the nonlinear dynamics of the populations induced by each pulse is measured as a function of inter-pulse delay by phase-sensitive detection with a lock-in amplifier. We focus on two limiting materials systems with contrasting optical properties: a prototypical lead-halide perovskite (LHP) solar cell, in which primary photoexcitations are charge photocarriers, and a single-component organic-semiconductor diode, which features Frenkel excitons as primary photoexcitations. The photoexcitation dynamics perceived by the two detection schemes in these contrasting systems are distinct. Nonlinear-dynamic contributions in the photoluminescence detection scheme arise from contributions to radiative recombination in both materials systems, while photocurrent arises directly in the LHP but indirectly following exciton dissociation in the organic system. Consequently, the basic photophysics of the two systems are reflected differently when comparing measurements with the two detection schemes. Our results indicate that photoluminescence detection in the LHP system provides valuable information about trap-assisted and Auger recombination processes, but that these processes are convoluted in a nontrivial way in the photocurrent response and are therefore difficult to differentiate. In contrast, the organic–semiconductor system exhibits more directly correlated responses in the nonlinear photoluminescence and photocurrent measurements, as charge carriers are secondary excitations only generated through exciton dissociation processes. We propose that bimolecular annihilation pathways mainly contribute to the generation of charge carriers in single-component organic semiconductor devices. Overall, our work highlights the utility of excitation correlation spectroscopy in modern semiconductor materials research, particularly in the analysis of nonlinear photophysical processes, which are deterministic for their electronic and optical properties.