AbstractMachine learning (ML) is gaining more attention in photovoltaic research and will be a vital tool in reaching record‐high power conversion efficiencies (PCE) in the near future. One area, where ML is significantly beneficial is reducing the number of experiments needed to find the optimum combination of parameters in solar cell fabrication. Bayesian optimization (BO) provides routes for quickly identifying optimum parameters in problems with large parameter space. In this work, BO algorithms utilizing previous knowledge are demonstrated to result in faster optimization of tandem solar cells, a technology rapidly gaining more interest due to its potential to deliver record‐high performance. Namely, it is shown that in the space of all possible parameter combinations that take ≈88 years to evaluate, optimum PCE can be obtained in 20 min. Moreover, it is demonstrated that methods utilizing previous knowledge outperform those that do not by yielding an increase of ≈8.9%abs. in the 1st iteration and requiring 5× less time to reach a target PCE of 38.5% across 20 different trials. Results from this work help accelerate the development of tandem solar cells by removing the need for large numbers of experiments in identifying optimum parameters.
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