Beyond Strain: Controlling the Surface Chemistry of CsPbI3 Nanocrystal Films for Improved Stability against Ambient Reactive Oxygen Species

Moot, Taylor; Dikova, Desislava R.; Hazarika, Abhijit; Schloemer, Tracy H.; Habisreutinger, Severin N.; Leick, Noemi; Dunfield, Sean P.; Rosales, Bryan A.; Harvey, Steven P.; Pfeilsticker, Jason R.; Teeter, Glenn; Wheeler, Lance M.; Larson, Bryon W.; Luther, Joseph M.

doi:10.1021/acs.chemmater.0c02543

Beyond Strain: Controlling the Surface Chemistry of CsPbI₃ Nanocrystal Films for Improved Stability against Ambient Reactive Oxygen Species

Journal Article · Mon Aug 31 00:00:00 EDT 2020 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.0c02543· OSTI ID:1762480

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National Renewable Energy Lab. (NREL), Golden, CO (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Michigan, Ann Arbor, MI (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States)
National Renewable Energy Laboratory, Golden, Colorado 80401, United States
National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)

Colloidal halide perovskite nanocrystals (NCs) have the possibility of easy scale-up due to their batch synthesis and have demonstrated excellent optoelectronic properties. In particular, perovskite NCs have remarkably high photoluminescence quantum yields in solution and as thin films and impressive open circuit voltages in photovoltaic devices. Despite these promising results, little work has been done to understand the stability of CsPbI₃ NCs for optoelectronic device applications. It has been previously shown that the ligands impart tensile surface strain, which stabilizes the black three-dimensional (3D) perovskite phase against phase degradation, making CsPbI₃ NCs some of the most structurally robust inorganic halide perovskites to date. However, understanding exactly how CsPbI₃ NCs degrade under ambient conditions is critical. Additionally, we demonstrate that the degradation mechanism of NCs is unique from, and 2 orders of magnitude slower than, their polycrystalline thin-film counterparts. Under specific conditions, CsPbI₃ NC films show a compositional instability instead of the phase instability seen in large grain CsPbI₃. This is mediated through reactions with superoxide and other reactive oxygen species, which are initiated from surface defect states, O₂ and light. We then use this mechanistic insight to identify multiple strategies to prolong the lifetimes of CsPbI₃ NC films, by going beyond surface strain to mitigate key surface chemistries. We demonstrate that (1) minimizing the number of surface defects (2) using an alkylammonium bromide ligand surface treatment and (3) encapsulation with an oxygen scavenging layer all increase NC film lifetimes by inhibiting various steps in the photo-oxidation degradation reaction.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Office of Workforce Development for Teachers and Scientists, Science Undergraduate Laboratory Internship (SULI) Program; USDOE National Renewable Energy Laboratory (NREL), Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Building Technologies Office (EE-5B)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1762480

Report Number(s):: NREL/JA--5900-76721; MainId:9382; UUID:3dfb7532-d9c7-4330-8239-504647d04edd; MainAdminID:19204

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 18 Vol. 32; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Beyond Strain: Controlling the Surface Chemistry of CsPbI3 Nanocrystal Films for Improved Stability against Ambient Reactive Oxygen Species

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