Decoupling Intrinsic Molecular Efficacy From Platform Effects: An Interpretable Machine Learning Framework for...

Area of Science:

• Materials Science
• Renewable Energy
• Computational Chemistry

Background:

• Designing effective interface passivators for perovskite solar cells is challenging due to the difficulty in distinguishing intrinsic molecular properties from device-specific performance factors.
• This complexity hinders the identification of truly novel chemical advancements in perovskite solar cell technology.

Purpose of the Study:

• To develop a generalizable and interpretable machine learning (ML) framework to decouple intrinsic molecular efficacy from extrinsic platform-dependent performance in perovskite solar cells.
• To enable the unbiased discovery of novel interface passivator molecules with genuine intrinsic performance gains.

Main Methods:

• An asymptotic saturation model was employed within an ML framework to analyze a dataset of 240 experimental entries.
• Key molecular descriptors, including hydrogen bond acceptor strength and electrostatic potential difference, were identified.
• A large-scale virtual screening of over 121 million PubChem compounds was conducted using diversity clustering and uncertainty quantification.

Main Results:

• The ML model successfully identified critical descriptors for intrinsic molecular efficacy.
• Five promising dual-functional passivator candidates (e.g., TDZ-S, TZC-F) were discovered with high predicted efficacy and confidence.
• First-principles calculations validated strong chemisorption, net electron donation, and optimized interfacial energetics for the identified candidates.

Conclusions:

• The developed ML framework provides a transferable paradigm for the rational design of materials by decoupling intrinsic and extrinsic factors.
• This approach accelerates the discovery of high-performance interface passivators for perovskite solar cells.
• The methodology is extendable to the design of materials for other optoelectronic interfaces beyond perovskite solar cells.