Conventional materials discovery is a laborious and time‐consuming process that can take decades from initial conception of the material to commercialization. Recent developments in materials acceleration platforms promise to accelerate materials discovery using automation of experiments coupled with machine learning. However, most of the automation efforts in chemistry focus on synthesis and compound identification, with integrated target property characterization receiving less attention. In this work, an automated platform is introduced for the discovery of molecules as gain mediums for organic semiconductor lasers, a problem that has been challenging for conventional approaches. This platform encompasses automated lego‐like synthesis, product identification, and optical characterization that can be executed in a fully integrated end‐to‐end fashion. Using this workflow to screen organic laser candidates, discovered eight potential candidates for organic lasers is discovered. The lasing threshold of four molecules in thin‐film devices and find two molecules with state‐of‐the‐art performance is tested. These promising results show the potential of automated synthesis and screening for accelerated materials development.

Accelerated Materials Discovery In article number 2207070, Tony C Wu, Alán Aspuru‐Guzik, and co‐workers report a materials acceleration platform to automatically search for high‐performing organic laser molecules, which includes synthesis, product identification, and property measurements. This platform has discovered two state‐of‐the‐art organic lasers from searching through 40 potential candidates. The results show the potential of automated synthesis and accelerated discovery of materials.

We investigated the impact of various excitonic and photonic losses on the lasing threshold and slope efficiency of organic semiconductor lasers (OSLs) under optical and electrical excitations. The rate equations are solved numerically using the Euler method for an OSL and an organic semiconductor laser diode (OSLD), including 4,4′-bis[(N-carbazole)styryl]biphenyl (BSB-Cz) as a gain medium. The results showed that the loss mechanisms that affect the exciton and photon densities cause an increase in the laser threshold and a decrease in the slope efficiency. Further, we demonstrated that by using a thermally activated delayed fluorescence (TADF) emitter as a gain medium, the triplet excitons could be harvested by increasing the reverse intersystem crossing rate (kRISC), resulting in an appreciable decrease of the laser threshold and an increase of the slope efficiency. Accordingly, the TADF emitters with a fast kRISC are expected to significantly reduce the current density required for electrical excitation.

In this study, electron and hole injection, and transport in semi-transparent organic light-emitting diodes, including dielectric/metal/dielectric (DMD) electrodes, were investigated. The DMD electrode was modified by incorporating a 5 nm-thick Cs:MoOx layer and a 10 nm-thick 1,4,5,8,9,11-hexaazatriphenylene hexacarbonitrile (HATCN) layer to improve the electron and hole injection in standard and inverse structures, respectively. The inverse structure showed a reasonably good and stable external quantum efficiency due to the well-balanced carrier densities at both low and high voltages which was confirmed by an electrical simulation study. Also, the peak position of the hole and electron recombination rate in the inverse structure was located on the ITO side, which is beneficial for reducing exciton quenching and photon absorption by metallic electrodes.

The control of laser emission angles in laser devices is essential for many optoelectronic and photonic applications such as optical sensing and displays. In this context, we studied the light diffraction pattern of laser beams in a one-dimensional sampled distributed feedback resonator having organic gain media. The gratings consist of the repetition of supercells having a mixed-order sampled grating in which 1st-order gratings surround a 2nd-order grating. The experimental results showed that the diffraction angles of the laser beams are quite diverse depending on the supercell structures. We demonstrate that the interval of the diffraction angle (θ) of the laser beams is inversely proportional to the length of the supercell experimentally and theoretically. By tuning the length of supercells as well as the length of 1st-order and 2nd-order regions, the interval θ was tuned from 0.1° to 43° with the different arc emission patterns. With the reduction of θ, i.e., the longer 1st-order region, a significant decrease in the laser threshold was obtained, resulting in the lowest lasing threshold of 2.5 ± 0.1  μJ/cm2 with ∼3.5 ns of a long pulse width excitation source.