Decoding the Broadband Emission of 2D Pb-Sn Halide Perovskites through High-Throughput Exploration

Foadian, Elham; Yang, Jonghee; Harris, Sumner B.; Tang, Yipeng; Rouleau, Christopher M.; Joy, Syed; Graham, Kenneth R.; Lawrie, Benjamin J.; Hu, Bin; Ahmadi, Mahshid

doi:10.1002/adfm.202411164

Decoding the Broadband Emission of 2D Pb-Sn Halide Perovskites through High-Throughput Exploration

Journal Article · Sat Aug 24 00:00:00 EDT 2024 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.202411164· OSTI ID:2491457

^[1]; ^[2]; Harris, Sumner B. ^[3]; Tang, Yipeng ^[1]; Rouleau, Christopher M. ^[3]; Joy, Syed ^[4]; Graham, Kenneth R. ^[4]; Lawrie, Benjamin J. ^[5]; Hu, Bin ^[1]; ^[1]

University of Tennessee, Knoxville, TN (United States)
University of Tennessee, Knoxville, TN (United States); Yonsei Univ., Seoul (Korea, Republic of)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Univ. of Kentucky, Lexington, KY (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Unlike single-component 2D metal halide perovskites (MHPs) exhibiting sharp excitonic photoluminescence (PL), a broadband PL emerges in mixed Pb-Sn 2D lattices. Two physical models –self-trapped exciton and defect-induced Stokes-shift – are proposed to explain this unconventional phenomenon. However, the explanations provide limited rationalizations without consideration of the formidable compositional space, and thus, the fundamental origin of broadband PL remains elusive. Herein, the high-throughput automated experimental workflow is established to systematically explore the broadband PL in mixed Pb-Sn 2D MHPs, employing PEA (Phenethylammonium) as a model cation known to work as a rigid organic spacer. Spectrally, the broadband PL becomes further broadened with rapid PEA₂PbI₄ phase segregation with increasing Pb concentrations during early-stage crystallization. Counterintuitively, MHPs with high Pb concentrations exhibit prolonged PL lifetimes. Hyperspectral microscopy identifies substantial PEA₂PbI₄ phase segregation in those films, hypothesizing that the establishment of charge transfer excitons by the phase segregation upon crystallization at high-Pb compositions results in distinctive PL properties. In conclusion, these results indicate that two independent mechanisms—defect-induced Stoke-shifts and the establishment of charge transfer excitons by phase segregation—coexist which significantly correlates with the Pb:Sn ratio, thereby simultaneously contributing to the broadband PL emission in 2D mixed Pb-Sn HPs.

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:: 2491457

Journal Information:: Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 52 Vol. 34; ISSN 1616-301X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Decoding the Broadband Emission of 2D Pb-Sn Halide Perovskites through High-Throughput Exploration

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