Active Learning Exploration of Transition-Metal Complexes to Discover Method-Insensitive and Synthetically Accessible Chromophores

Transition-metal chromophores with earth -abundant transition metals are an important design target for their applications in lighting and nontoxic bioimaging, but their design is challenged by the scarcity of complexes that simultaneously have well-defined ground states and optimal target absorption energies in the visible region. Machine learning (ML) accelerated discovery could overcome such challenges by enabling the screening of a larger space but is limited by the fidelity of the data used in ML model training, which is typically from a single approximate density functional. To address this limitation, we search for consensus in predictions among 23 density functional approximations across multiple rungs of "Jacob's ladder". To accelerate the discovery of complexes with absorption energies in the visible region while minimizing the effect of low-lying excited states, we use two-dimensional (2D)efficient global optimization to sample candidate low spin chromophores from multimillion complex spaces. Despite the scarcity (i.e., similar to 0.01%) of potential chromophores in this large chemical space, we identify candidates with high likelihood (i.e., >10%) of computational validation as the ML models improve during active learning, representing a 1000-fold acceleration in discovery. Absorption spectra of promising chromophores from time dependent density functional theory verify that 2/3 of candidates have the desired excited-state properties. The observation that constituent ligands from our leads have demonstrated interesting optical properties in the literature exemplifies the effectiveness of our construction of a realistic design space and active learning approach.