Metal Halide Perovskites Demonstrate Radiation Hardness and Defect Healing in Vacuum

Holland, Michael; Ruth, Anthony; Mielczarek, Kamil; Dhas, Vivek V.; Berry, Joseph J.; Irwin, Michael D.

doi:10.1021/acsami.1c24709

Title: Metal Halide Perovskites Demonstrate Radiation Hardness and Defect Healing in Vacuum

Journal Article · 10 February 2022 · ACS Applied Materials and Interfaces

DOI: https://doi.org/10.1021/acsami.1c24709 · OSTI ID:1846751

^[1]; Ruth, Anthony ^[1]; Mielczarek, Kamil ^[1]; Dhas, Vivek V. ^[1];

^[2]; Irwin, Michael D. ^[1]

CubicPV Inc., Dallas, TX (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States)

Herein, we subject formamidinium lead iodide films to oxygen-containing gases (flowing O₂ or free diffusion of lab atmosphere), inert gases (flowing He, Ar, or N₂), and vacuum. Our films are irradiated by Cu Ka X-rays and held at 75 °C while X-ray diffraction is recorded. Under all gas conditions, we observe a reproducible 1.1 ± 0.5 A³ perovskite lattice contraction from an initial unit cell volume of 256.5 ± 0.8 A³ concurrent with continuous perovskite loss and lead iodide growth. Oxygen-containing gases increase the reaction rates without materially altering perovskite structural changes. Under the same temperature and irradiation conditions in vacuo, a self-healing reaction is observed, exhibited by a reproducible (0.9 ± 0.3 A³) lattice expansion and stabilization of the perovskite. Furthermore, interactions between the perovskite, defects, and minority phases are simulated by generalized gradient approximation Perdew-Burke-Ernzerhof (GGA-PBE) density functional theory. Lattice contraction indicates an increase in the concentration of Schottky defects-pairs of formamidinium and iodine vacancies. Under irradiation in every atmospheric condition, a solid solution of Schottky defects with a concentration of several percent diffuses and precipitates forming lead iodide and consuming the defects. In the presence of ionized gases, this framework is modified to include the continual loss of formamidinium and iodine ions from the perovskite forming Schottky defects.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1846751

Report Number(s):: NREL/JA-5K00-78648; MainId:32565; UUID:90051357-fa4b-4800-8424-bed0fa7b8c6b; MainAdminID:63926

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 7 Vol. 14; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

14 SOLAR ENERGY
36 MATERIALS SCIENCE
Schottky defects
X-ray diffraction
defects
degradation
environmental degradation
in vacuo
ion migration
lattices
perovskites
photovoltaics
vacuum

Title: Metal Halide Perovskites Demonstrate Radiation Hardness and Defect Healing in Vacuum

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