Vacancy-Mediated Anion Photosegregation Kinetics in Mixed Halide Hybrid Perovskites: Coupled Kinetic Monte Carlo and Optical Measurements

Ruth, Anthony; Brennan, Michael C.; Draguta, Sergiu; Morozov, Yurii V.; Zhukovskyi, Maksym; Janko, Boldizsar; Zapol, Peter; Kuno, Masaru

doi:10.1021/acsenergylett.8b01369

Title: Vacancy-Mediated Anion Photosegregation Kinetics in Mixed Halide Hybrid Perovskites: Coupled Kinetic Monte Carlo and Optical Measurements

Journal Article · Wed Sep 05 00:00:00 EDT 2018 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.8b01369· OSTI ID:1489373

Ruth, Anthony ^[1]; Brennan, Michael C. ^[2]; Draguta, Sergiu ^[2]; Morozov, Yurii V. ^[2]; Zhukovskyi, Maksym ^[2]; Janko, Boldizsar ^[1];

^[3];

^[4]

Univ. of Notre Dame, Notre Dame, IN (United States). Dept. of Physics
Univ. of Notre Dame, Notre Dame, IN (United States). Dept. of Chemistry and Biochemistry
Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Div.
Univ. of Notre Dame, Notre Dame, IN (United States). Dept. pf Physics and Dept. of Chemistry and Biochemistry

Solution-processed mixed halide perovskites are excellent materials for multijunction solar cells. Unfortunately, light-induced halide phase segregation has prevented their effective integration into working devices. In this study, we rationalize and quantify anion photosegregation in stoichiometric and halide-deficient MAPb(I1–xBrx)3 thin films through kinetic Monte Carlo simulations and complementary optical measurements. Our study reveals that segregation rates are dictated by halide vacancy hopping barriers and are modulated by vacancy concentrations. The simulations further suggest that near-ubiquitous emission energies, which converge on that for MAPb(I0.8Br0.2)3 (i.e., x ≈ 0.2) following photosegregation, arise from the existence of kinetically trapped Br– within nucleated I-rich domains. An established photosegregation excitation intensity threshold is independent of the number of vacancies and instead depends critically on parameters such as carrier diffusion length, lifetime, and bandgap tunability. The study thus sheds new light on important parameters that define halide photosegregation and presents opportunities for controlling the phenomenon.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); University of Notre Dame, IN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; SC0014334

OSTI ID:: 1489373

Alternate ID(s):: OSTI ID: 1657799

Journal Information:: ACS Energy Letters, Vol. 3, Issue 10; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 87 works

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