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Local nanoscale phase impurities are degradation sites in halide perovskites.

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cam.depositDate2022-05-25
cam.issuedOnline2022-05-24
cam.orpheus.success2022-05-25 - Embargo set during processing via Fast-track
datacite.issupplementedby.urlhttps://doi.org/10.17863/CAM.85310
dc.contributor.authorMacpherson, Stuart
dc.contributor.authorDoherty, Tiarnan AS
dc.contributor.authorWinchester, Andrew J
dc.contributor.authorKosar, Sofiia
dc.contributor.authorJohnstone, Duncan N
dc.contributor.authorChiang, Yu-Hsien
dc.contributor.authorGalkowski, Krzysztof
dc.contributor.authorAnaya, Miguel
dc.contributor.authorFrohna, Kyle
dc.contributor.authorIqbal, Affan N
dc.contributor.authorNagane, Satyawan
dc.contributor.authorRoose, Bart
dc.contributor.authorAndaji-Garmaroudi, Zahra
dc.contributor.authorOrr, Kieran WP
dc.contributor.authorParker, Julia E
dc.contributor.authorMidgley, Paul A
dc.contributor.authorDani, Keshav M
dc.contributor.authorStranks, Samuel D
dc.contributor.orcidDoherty, Tiarnan AS [0000-0003-1150-4012]
dc.contributor.orcidChiang, Yu-Hsien [0000-0003-2767-3056]
dc.contributor.orcidAnaya, Miguel [0000-0002-0384-5338]
dc.contributor.orcidFrohna, Kyle [0000-0002-2259-6154]
dc.contributor.orcidIqbal, Affan N [0000-0002-7582-9011]
dc.contributor.orcidNagane, Satyawan [0000-0002-1146-4754]
dc.contributor.orcidRoose, Bart [0000-0002-0972-1475]
dc.contributor.orcidOrr, Kieran WP [0000-0001-9996-1458]
dc.contributor.orcidDani, Keshav M [0000-0003-3917-6305]
dc.contributor.orcidStranks, Samuel D [0000-0002-8303-7292]
dc.date.accessioned2022-05-25T23:31:00Z
dc.date.available2022-05-25T23:31:00Z
dc.date.issued2022-07
dc.date.updated2022-05-25T09:49:49Z
dc.description.abstractUnderstanding the nanoscopic chemical and structural changes that drive instabilities in emerging energy materials is essential for mitigating device degradation. The power conversion efficiency of halide perovskite photovoltaic devices has reached 25.7 per cent in single-junction and 29.8 per cent in tandem perovskite/silicon cells1,2, yet retaining such performance under continuous operation has remained elusive3. Here we develop a multimodal microscopy toolkit to reveal that in leading formamidinium-rich perovskite absorbers, nanoscale phase impurities, including hexagonal polytype and lead iodide inclusions, are not only traps for photoexcited carriers, which themselves reduce performance4,5, but also, through the same trapping process, are sites at which photochemical degradation of the absorber layer is seeded. We visualize illumination-induced structural changes at phase impurities associated with trap clusters, revealing that even trace amounts of these phases, otherwise undetected with bulk measurements, compromise device longevity. The type and distribution of these unwanted phase inclusions depends on the film composition and processing, with the presence of polytypes being most detrimental for film photo-stability. Importantly, we reveal that both performance losses and intrinsic degradation processes can be mitigated by modulating these defective phase impurities, and demonstrate that this requires careful tuning of local structural and chemical properties. This multimodal workflow to correlate the nanoscopic landscape of beam-sensitive energy materials will be applicable to a wide range of semiconductors for which a local picture of performance and operational stability has yet to be established.
dc.identifier.doi10.17863/CAM.84907
dc.identifier.eissn1476-4687
dc.identifier.issn0028-0836
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/337493
dc.language.isoeng
dc.publisherSpringer Science and Business Media LLC
dc.publisher.departmentDepartment of Physics
dc.publisher.departmentDepartment of Chemical Engineering And Biotechnology
dc.publisher.urlhttp://dx.doi.org/10.1038/s41586-022-04872-1
dc.rightsAll Rights Reserved
dc.rights.urihttp://www.rioxx.net/licenses/all-rights-reserved
dc.subject3403 Macromolecular and Materials Chemistry
dc.subject40 Engineering
dc.subject34 Chemical Sciences
dc.subject3406 Physical Chemistry
dc.subject7 Affordable and Clean Energy
dc.titleLocal nanoscale phase impurities are degradation sites in halide perovskites.
dc.typeArticle
dcterms.dateAccepted2022-05-13
prism.publicationNameNature
pubs.funder-project-idRoyal Society (UF150033)
pubs.funder-project-idEuropean Research Council (756962)
pubs.funder-project-idEuropean Commission Horizon 2020 (H2020) Marie Sk?odowska-Curie actions (841136)
pubs.funder-project-idEuropean Commission Horizon 2020 (H2020) Marie Sk?odowska-Curie actions (841386)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/S030638/1)
pubs.funder-project-idEPSRC (EP/T02030X/1)
pubs.funder-project-idEPSRC (2127077)
pubs.funder-project-idEPSRC (EP/V012932/1)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/R023980/1)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/R008779/1)
pubs.funder-project-idEuropean Commission Horizon 2020 (H2020) Research Infrastructures (RI) (823717)
pubs.funder-project-idEPSRC (EP/V007750/1)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/P007767/1)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/P024947/1)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/R00661X/1)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/S019367/1)
pubs.funder-project-idEPSRC (via University of Manchester) (EP/X527257/1)
pubs.licence-display-nameApollo Repository Deposit Licence Agreement
pubs.licence-identifierapollo-deposit-licence-2-1
rioxxterms.typeJournal Article/Review
rioxxterms.versionAM
rioxxterms.versionofrecord10.1038/s41586-022-04872-1

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