Temperature Dependence of the Energy Levels of Methylammonium Lead Iodide Perovskite from First-Principles.
dc.contributor.author | Saidi, Wissam A | |
dc.contributor.author | Poncé, Samuel | |
dc.contributor.author | Monserrat, Bartomeu | |
dc.date.accessioned | 2018-11-21T00:30:34Z | |
dc.date.available | 2018-11-21T00:30:34Z | |
dc.date.issued | 2016-12-15 | |
dc.identifier.issn | 1948-7185 | |
dc.identifier.uri | https://www.repository.cam.ac.uk/handle/1810/285508 | |
dc.description.abstract | Environmental effects and intrinsic energy-loss processes lead to fluctuations in the operational temperature of solar cells, which can profoundly influence their power conversion efficiency. Here we determine from first-principles the effects of temperature on the band gap and band edges of the hybrid pervoskite CH3NH3PbI3 by accounting for electron-phonon coupling and thermal expansion. From 290 to 380 K, the computed band gap change of 40 meV coincides with the experimental change of 30-40 meV. The calculation of electron-phonon coupling in CH3NH3PbI3 is particularly intricate as the commonly used Allen-Heine-Cardona theory overestimates the band gap change with temperature, and excellent agreement with experiment is only obtained when including high-order terms in the electron-phonon interaction. We also find that spin-orbit coupling enhances the electron-phonon coupling strength but that the inclusion of nonlocal correlations using hybrid functionals has little effect. We reach similar conclusions in the metal-halide perovskite CsPbI3. Our results unambiguously confirm for the first time the importance of high-order terms in the electron-phonon coupling by direct comparison with experiment. | |
dc.format.medium | Print-Electronic | |
dc.language | eng | |
dc.publisher | American Chemical Society (ACS) | |
dc.title | Temperature Dependence of the Energy Levels of Methylammonium Lead Iodide Perovskite from First-Principles. | |
dc.type | Article | |
prism.endingPage | 5252 | |
prism.issueIdentifier | 24 | |
prism.publicationDate | 2016 | |
prism.publicationName | J Phys Chem Lett | |
prism.startingPage | 5247 | |
prism.volume | 7 | |
dc.identifier.doi | 10.17863/CAM.32866 | |
dcterms.dateAccepted | 2016-12-03 | |
rioxxterms.versionofrecord | 10.1021/acs.jpclett.6b02560 | |
rioxxterms.licenseref.uri | http://www.rioxx.net/licenses/all-rights-reserved | |
rioxxterms.licenseref.startdate | 2016-12-07 | |
dc.contributor.orcid | Saidi, Wissam A [0000-0001-6714-4832] | |
dc.identifier.eissn | 1948-7185 | |
rioxxterms.type | Journal Article/Review | |
cam.issuedOnline | 2016-12-07 | |
rioxxterms.freetoread.startdate | 2017-12-07 |
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