Repository logo
 

Dedoping of Lead Halide Perovskites Incorporating Monovalent Cations.

Simple item page
cam.issuedOnline2018-07-06
datacite.issupplementedby.urlhttps://www.repository.cam.ac.uk/handle/1810/278386
dc.contributor.authorAbdi-Jalebi, Mojtaba
dc.contributor.authorPazoki, Meysam
dc.contributor.authorPhilippe, Bertrand
dc.contributor.authorDar, M Ibrahim
dc.contributor.authorAlsari, Mejd
dc.contributor.authorSadhanala, Aditya
dc.contributor.authorDivitini, Giorgio
dc.contributor.authorImani, Roghayeh
dc.contributor.authorLilliu, Samuele
dc.contributor.authorKullgren, Jolla
dc.contributor.authorRensmo, Håkan
dc.contributor.authorGrätzel, Michael
dc.contributor.authorFriend, Richard H
dc.contributor.orcidAbdi-Jalebi, Mojtaba [0000-0002-9430-6371]
dc.contributor.orcidPazoki, Meysam [0000-0001-6776-5460]
dc.contributor.orcidPhilippe, Bertrand [0000-0003-2412-8503]
dc.contributor.orcidDar, M Ibrahim [0000-0001-9489-8365]
dc.contributor.orcidSadhanala, Aditya [0000-0003-2832-4894]
dc.contributor.orcidLilliu, Samuele [0000-0002-8449-2211]
dc.contributor.orcidKullgren, Jolla [0000-0003-3570-0050]
dc.contributor.orcidGrätzel, Michael [0000-0002-0068-0195]
dc.contributor.orcidFriend, Richard H [0000-0001-6565-6308]
dc.date.accessioned2018-07-04T12:31:14Z
dc.date.available2018-07-04T12:31:14Z
dc.date.issued2018-07-24
dc.description.abstractWe 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.
dc.description.sponsorshipCambridge Materails Limited, Nava Technology Limited
dc.format.mediumPrint-Electronic
dc.identifier.doi10.17863/CAM.25141
dc.identifier.eissn1936-086X
dc.identifier.issn1936-0851
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/277802
dc.languageeng
dc.language.isoeng
dc.publisherAmerican Chemical Society (ACS)
dc.publisher.urlhttp://dx.doi.org/10.1021/acsnano.8b03586
dc.subjectdedoped perovskite thin films
dc.subjectenhanced optoelectronic quality
dc.subjectinterstitial doping
dc.subjectmonovalent cations
dc.subjectsubstitutional doping
dc.titleDedoping of Lead Halide Perovskites Incorporating Monovalent Cations.
dc.typeArticle
dcterms.dateAccepted2018-06-28
prism.endingPage7311
prism.issueIdentifier7
prism.publicationDate2018
prism.publicationNameACS Nano
prism.startingPage7301
prism.volume12
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/M005143/1)
rioxxterms.licenseref.startdate2018-07-06
rioxxterms.licenseref.urihttp://www.rioxx.net/licenses/all-rights-reserved
rioxxterms.typeJournal Article/Review
rioxxterms.versionAM
rioxxterms.versionofrecord10.1021/acsnano.8b03586

Files

Original bundle
Now showing 1 - 2 of 2
No Thumbnail Available
Name:
Main, Dedoped Pk, vFinal.docx
Size:
6.2 MB
Format:
Microsoft Word XML
Description:
Accepted version
Licence
http://www.rioxx.net/licenses/all-rights-reserved
Download
No Thumbnail Available
Name:
SI, Dedoped Pk, vFinal.docx
Size:
10.98 MB
Format:
Microsoft Word XML
Description:
Supporting information
Licence
http://www.rioxx.net/licenses/all-rights-reserved
Download
License bundle
Now showing 1 - 1 of 1
No Thumbnail Available
Name:
DepositLicenceAgreement.pdf
Size:
417.78 KB
Format:
Adobe Portable Document Format
Download

Collections

Scholarly Works - Materials Science and Metallurgy