Simultaneous Optimization of Efficiency and Degradation in Tunable HTL-Free Perovskite Solar Cells with MWCNT-Integrated Back Contact Using a Machine Learning-Derived Polynomial Regressor

Abstract

Perovskite solar cells (PSCs) without a hole transport layer (HTL) offer a cost-effective and stable alternative to conventional architectures, utilizing only an absorber layer and an electron transport layer (ETL). This study presents a machine learning (ML)-driven framework to optimize the efficiency and stability of HTL-free PSCs by integrating experimental validation with numerical simulations. Excellent agreement is achieved between a fabricated device and its simulated counterpart at a molar fraction \( x = 68.7\% \) in \(\mathrm{MAPb}_{1-x}\mathrm{Sb}_{2x/3}\mathrm{I}_3\), where MA is methylammonium. A dataset of 1650 samples is generated by varying molar fraction, absorber defect density, thickness, and ETL doping, with corresponding efficiency and 50-hour degradation as targets. A fourth-degree polynomial regressor (PR-4) shows the best performance, achieving RMSEs of 0.0179 and 0.0117, and \( R^2 \) scores of 1 and 0.999 for efficiency and degradation, respectively. The derived model generalizes beyond the training range and is used in an L-BFGS-B optimization algorithm with a weighted objective function to maximize efficiency and minimize degradation. This improves device efficiency from 13.7\% to 16.84\% and reduces degradation from 6.61\% to 2.39\% over 1000 hours. Finally, the dataset is labeled into superior and inferior classes, and a multilayer perceptron (MLP) classifier achieves 100\% accuracy, successfully identifying optimal configurations.