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Dedoping of Lead Halide Perovskites Incorporating Monovalent Cations
Univ Cambridge, Dept Phys, Cavendish Lab, JJ Thomson Ave, Cambridge, England.
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Tekniska sektionen, Institutionen för teknikvetenskaper, Fasta tillståndets fysik.ORCID-id: 0000-0001-6776-5460
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Fysiska sektionen, Institutionen för fysik och astronomi, Molekyl- och kondenserade materiens fysik.ORCID-id: 0000-0003-2412-8503
Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Lab Photon & Interfaces, Lausanne, Switzerland.
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2018 (Engelska)Ingår i: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 12, nr 7, s. 7301-7311Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

We report significant improvements in the optoelectronic properties of lead halide perovskites with the addition of monovalent ions with ionic radii close to Pb2+. We investigate the chemical distribution and electronic structure of solution processed CH3NH3PbI3 perovskite structures containing Na+, Cu+, and Ag+, which are lower valence metal ions than Pb2+ but have similar ionic radii. Synchrotron X-ray diffraction reveals a pronounced shift in the main perovskite peaks for the monovalent cation-based films, suggesting incorporation of these cations into the perovskite lattice as well as a preferential crystal growth in Ag+ containing perovskite structures. Furthermore, the synchrotron X-ray photoelectron measurements show a significant change in the valence band position for Cu- and Ag-doped films, although the perovskite bandgap remains the same, indicating a shift in the Fermi level position toward the middle of the bandgap. Such a shift infers that incorporation of these monovalent cations dedope the n-type perovskite films when formed without added cations. This dedoping effect leads to cleaner bandgaps as reflected by the lower energetic disorder in the monovalent cation-doped perovskite thin films as compared to pristine films. We also find that in contrast to Ag+ and Cu+, Na+ locates mainly at the grain boundaries and surfaces. Our theoretical calculations confirm the observed shifts in X-ray diffraction peaks and Fermi level as well as absence of intrabandgap states upon energetically favorable doping of perovskite lattice by the monovalent cations. We also model a significant change in the local structure, chemical bonding of metal-halide, and the electronic structure in the doped perovskites. In summary, our work highlights the local chemistry and influence of monovalent cation dopants on crystallization and the electronic structure in the doped perovskite thin films.

Ort, förlag, år, upplaga, sidor
2018. Vol. 12, nr 7, s. 7301-7311
Nyckelord [en]
monovalent cations, dedoped perovskite thin films, enhanced optoelectronic quality, substitutional doping, interstitial doping
Nationell ämneskategori
Materialkemi Teknik och teknologier
Identifikatorer
URN: urn:nbn:se:uu:diva-364505DOI: 10.1021/acsnano.8b03586ISI: 000440505000097PubMedID: 29953817OAI: oai:DiVA.org:uu-364505DiVA, id: diva2:1260751
Forskningsfinansiär
VetenskapsrådetEnergimyndighetenStiftelsen för strategisk forskning (SSF)StandUpEU, Horisont 2020, 687008Swedish National Infrastructure for Computing (SNIC), snice 2017-01-15; snice 2016-10-23Tillgänglig från: 2018-11-05 Skapad: 2018-11-05 Senast uppdaterad: 2019-02-19Bibliografiskt granskad

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