Accelerated screening of functional atomic impurities in halide perovskites using high-throughput computations and machine learning

Arun Mannodi-Kanakkithodi*, Maria K.Y. Chan

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

18 Scopus citations

Abstract

The pressing need for novel materials that can serve rising demands in solar cell and optoelectronic technologies makes the nexus of halide perovskites, high-throughput computations, and machine learning, very promising. Ever increasing amounts of data on the structure, fundamental properties, and device performance of halide perovskites provide opportunities for learning chemical rules and design principles that make these materials attractive, and applying them across wide chemical spaces. In this work, we show that impurity properties of halide perovskites computed using density functional theory (DFT) can be combined with machine learning (ML) to deliver predictive models and quick identification of optoelectronically active impurity atoms. Our computation lead to the largest reported dataset of the formation energies and charge transition levels of Pb-site impurities in methylammonium lead halide (MAPbX 3) perovskites. Descriptors are defined to uniquely represent any impurity atom in any MAPbX 3 compound and mapped to the computed impurity properties using regression techniques such as Gaussian process regression, neural networks, and random forests. We use the best optimized predictive models to make predictions for hundreds of impurities across 9 MAPbX 3 compounds and create lists of dominating impurities, that is, impurities that can shift the equilibrium Fermi level in the perovskite as determined by native point defects. This accelerated screening powered by computations and machine learning can guide the identification of problematic impurities that may cause undesired recombination of charge carriers, as well as impurities that can be deliberately introduced to tune the perovskite conductivity and resulting photovoltaic absorption.

Original languageEnglish (US)
Pages (from-to)10736-10754
Number of pages19
JournalJournal of Materials Science
Volume57
Issue number23
DOIs
StatePublished - Jun 2022

Funding

Extensive discussions with and scientific feedback from Dr. Alex Martinson (Argonne), Dr. David Fenning (UCSD), Rishi Kumar (UCSD), and Dr. Ji-Sang Park (Kyungpook National University) are acknowledged. This work was performed, partly at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357, and partly at Purdue University, under startup account number F.10023800.05.002. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. We gratefully acknowledge the computing resources provided on Bebop, a high-performance computing cluster operated by the Laboratory Computing Resource Center at Argonne National Laboratory.

ASJC Scopus subject areas

  • Ceramics and Composites
  • Materials Science (miscellaneous)
  • General Materials Science
  • Mechanics of Materials
  • Mechanical Engineering
  • Polymers and Plastics

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