Excitation Intensity- and Size-Dependent Halide Photosegregation in CsPb(I0.5Br0.5)3 Perovskite Nanocrystals

Gushchina, Irina; Trepalin, Vadim; Zaitsev, Evgenii; Ruth, Anthony; Kuno, Masaru

doi:10.1021/acsnano.2c10781

Excitation Intensity- and Size-Dependent Halide Photosegregation in CsPb(I_0.5Br_0.5)₃ Perovskite Nanocrystals

Journal Article · Sun Dec 04 23:00:00 EST 2022 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.2c10781· OSTI ID:1909224

^[1]; Trepalin, Vadim ^[2]; Zaitsev, Evgenii ^[2]; Ruth, Anthony ^[3]; ^[2]

Univ. of Notre Dame, IN (United States); University of Notre Dame
Univ. of Notre Dame, IN (United States)
CubicPV, Dallas, TX (United States)

Although broad consensus exists that photoirradiation of mixed-halide lead perovskites leads to anion segregation, no model today fully rationalizes all aspects of this near ubiquitous phenomenon. In this work, we quantitatively compare experimental, CsPb(I_0.5Br_0.5)₃ nanocrystal (NC) terminal anion photosegregation stoichiometries and excitation intensity thresholds to a band gap-based, thermodynamic model of mixed-halide perovskite photosegregation. Mixed-halide NCs offer strict tests of theory given physical sizes, which dictate local photogenerated carrier densities. We observe that mixed-anion perovskite NCs exhibit significant robustness to photosegregation, with photosegregation propensity decreasing with decreasing NC size. Observed size- and excitation intensity-dependent photosegregation data agree with model predicted size- and excitation intensity-dependent terminal halide stoichiometries. Established correspondence between experiment and theory, in turn, suggests that mixed-halide perovskite photostabilities can be predicted a priori using local gradients of (empirical) Vegard’s law expressions of composition-dependent band gaps.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Notre Dame, IN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0014334

OSTI ID:: 1909224

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 12 Vol. 16; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Excitation Intensity- and Size-Dependent Halide Photosegregation in CsPb(I0.5Br0.5)3 Perovskite Nanocrystals

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Excitation Intensity- and Size-Dependent Halide Photosegregation in CsPb(I_0.5Br_0.5)₃ Perovskite Nanocrystals