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Frustrated Lewis pair-mediated recrystallization of CH3NH3PbI3 for improved optoelectronic quality and high voltage planar perovskite solar cells
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Swansea Univ Bay Campus, Coll Engn, SPECIFIC, Fabian Way, Swansea SA1 8EN, W Glam, Wales.
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
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2016 (English)In: Energy & Environmental Science, ISSN 1754-5692, E-ISSN 1754-5706, Vol. 9, no 12, p. 3770-3782Article in journal (Refereed) Published
Abstract [en]

Films of the hybrid lead halide perovskite CH3NH3PbI3 were found to react with pyridine vapor at room temperature leading to complete bleaching of the film. In dry air or nitrogen atmosphere recrystallization takes place, leading to perovskite films with markedly improved optical and photovoltaic properties. The physical and chemical origin of the reversible bleaching and recrystallization mechanism was investigated using a variety of experimental techniques and quantum chemical calculations. The strong Lewis base pyridine attacks the CH3NH3PbI3. The mechanism can be understood from a frustrated Lewis pair formation with a partial electron donation of the lone-pair on nitrogen together with competitive bonding to other species as revealed by Raman spectroscopy and DFT calculations. The bleached phase consists of methylammonium iodide crystals and an amorphous phase of PbI2( pyridine)(2). After spontaneous recrystallization the CH3NH3PbI3 thin films have remarkably improved photoluminescence, and solar cell performance increased from 9.5% for as-deposited films to more than 18% power conversion efficiency for recrystallized films in solar cells with planar geometry under AM1.5G illumination. Hysteresis was negligible and open-circuit potential was remarkably high, 1.15 V. The results show that complete recrystallization can be achieved with a simple room temperature pyridine vapor treatment of CH3NH3PbI3 films leading to high quality crystallinity films with drastically improved photovoltaic performance.

Place, publisher, year, edition, pages
2016. Vol. 9, no 12, p. 3770-3782
National Category
Physical Chemistry Engineering and Technology
Research subject
Physics with spec. in Atomic, Molecular and Condensed Matter Physics
Identifiers
URN: urn:nbn:se:uu:diva-311577DOI: 10.1039/c6ee02544gISI: 000392915500017OAI: oai:DiVA.org:uu-311577DiVA, id: diva2:1060689
Funder
Swedish Energy AgencyStandUpSwedish Research CouncilGöran Gustafsson Foundation for promotion of scientific research at Uppala University and Royal Institute of TechnologyKnut and Alice Wallenberg FoundationAvailable from: 2016-12-29 Created: 2016-12-29 Last updated: 2017-11-29Bibliographically approved

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Jain, Sagar MotilalQiu, ZhenHäggman, LeifMirmohades, MohammadJohansson, Malin B.Edvinsson, TomasBoschloo, Gerrit

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