Compositional heterogeneity in CsyFA1-yPb(BrxI1-x)3 perovskite films and its impact on phase behavior

Barrier, Julien; Beal, Rachel E.; Gold-Parker, Aryeh; Vigil, Julian A.; Wolf, Eli; Waquier, Louis; Weadock, Nicholas J.; Zhang, Zihan; Schelhas, Laura T.; Nogueira, Ana Flavia; McGehee, Michael D.; Toney, Michael F.

doi:10.1039/d1ee01184g

Title: Compositional heterogeneity in Cs_yFA_1-yPb(Br_xI_1-x)₃ perovskite films and its impact on phase behavior

Journal Article · Mon Oct 11 00:00:00 EDT 2021 · Energy & Environmental Science

DOI:https://doi.org/10.1039/d1ee01184g· OSTI ID:1873377

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^[3]; Waquier, Louis ^[1];

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SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL); Ecole Superieure de Physique et de Chimie Industrielles (ESPCI), ParisTech (France)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL); Stanford Univ., CA (United States)
Stanford Univ., CA (United States); Univ. of Colorado, Boulder, CO (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL); Univ. of Colorado, Boulder, CO (United States)
Univ. of Colorado, Boulder, CO (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Univ. of Campinas (UNICAMP), Sao Paulo (Brazil)
Univ. of Colorado, Boulder, CO (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)

Hybrid organic inorganic lead halide perovskite semiconductors of the form Cs_yFA_1-yPb(Br_xI_1-x)₃ are promising candidate materials for high-efficiency photovoltaics. Notably, cation and anion substitution can be used to tune the band gaps to optimize performance and improve stability. However, multi-component materials can be prone to compositional and structural inhomogeneity and the extent, length scale and impact of this heterogeneity on lead halide perovskite properties are not well understood. Here we use synchrotron X-ray diffraction to probe the evolution of crystal structure across the tetragonal-to-cubic phase transition for a series of Cs_yFA_1-yPb(Br_xI_1-x)₃ thin films with x = 0.05 to 0.3 and y = 0.17 to 0.40. We find that the transition occurs across a broad temperature range of approximately 40 °C, much larger than for pure compounds such as MAPbI₃ and MAPbBr₃. Finally, we hypothesize that this smearing of the phase transition is due to compositional inhomogeneities that give rise to a distribution of local transition temperatures and we estimate the composition varies by about 10% to 15% with likely greater heterogeneity for the halide anion than the cation. This approach of mapping the transition is a simple and effective method of assessing heterogeneity, enabling evaluation of its impact.

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Research Organization:: SLAC National Accelerator Lab., Menlo Park, CA (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: AC36-08-GO28308; AC02-76SF00515; ECCS-2026822; DGE–1656518; AC36-08GO28308

OSTI ID:: 1873377

Alternate ID(s):: OSTI ID: 1827446; OSTI ID: 1840711

Report Number(s):: NREL/JA-5900-81868; 1656518; ECCS-2026822; TRN: US2307014

Journal Information:: Energy & Environmental Science, Vol. 14, Issue 12; ISSN 1754-5692

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
crystal structure
energy gap
lead compounds
organic-inorganic materials
perovskite
x-ray diffraction

Title: Compositional heterogeneity in CsyFA1-yPb(BrxI1-x)3 perovskite films and its impact on phase behavior

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References (65)

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Title: Compositional heterogeneity in Cs_yFA_1-yPb(Br_xI_1-x)₃ perovskite films and its impact on phase behavior