High-Throughput Automated Exploration of Phase Growth Behaviors in Quasi-2D Formamidinium Metal Halide Perovskites

Yang, Jonghee; Lawrie, Benjamin J.; Kalinin, Sergei V.; Ahmadi, Mahshid

doi:10.1002/aenm.202302337

High-Throughput Automated Exploration of Phase Growth Behaviors in Quasi-2D Formamidinium Metal Halide Perovskites

Journal Article · Sun Sep 24 00:00:00 EDT 2023 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202302337· OSTI ID:2006941

^[1]; ^[2]; Kalinin, Sergei V. ^[1]; ^[1]

Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Quasi-2D metal halide perovskites (MHPs) are an emerging material platform for sustainable functional optoelectronics, but the uncontrollable, broad phase distribution remains a critical challenge for applications. Nevertheless, the basic principles for controlling phases in quasi-2D MHPs remain poorly understood, due to the rapid crystallization kinetics during the conventional thin-film fabrication process. In this work, a high-throughput automated synthesis-characterization-analysis workflow is implemented to accelerate material exploration in formamidinium (FA)-based quasi-2D MHP compositional space, revealing the early-stage phase growth behaviors fundamentally determining the phase distributions. Upon comprehensive exploration with varying synthesis conditions including 2D:3D composition ratios, antisolvent injection rates, and temperatures in an automated synthesis-characterization platform, it is observed that the prominent n = 2 2D phase restricts the growth kinetics of 3D-like phases—α-FAPbI₃ MHPs with spacer-coordinated surface—across the MHP compositions. Thermal annealing is a critical step for proper phase growth, although it can lead to the emergence of unwanted local PbI₂ crystallites. Additionally, fundamental insights into the precursor chemistry associated with spacer-solvent interaction determining the quasi-2D MHP morphologies and microstructures are demonstrated. The high-throughput study provides comprehensive insights into the fundamental principles in quasi-2D MHP phase control, enabling new control of the functionalities in complex materials systems for sustainable device applications.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: Alfred P. Sloan Foundation; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2006941

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 43 Vol. 13; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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