Methodological Issues in first-principle calculations of CH3NH3PbI3 perovskite surfaces: Quantum confinement and thermal motion
Author
dc.contributor.author
Lodeiro, Lucas
Author
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Barría Cáceres, Felipe
Author
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Jiménez, Karla
Author
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Contreras, Renato
Author
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Montero Alejo, Ana L.
Author
dc.contributor.author
Menéndez Proupin, Eduardo
Admission date
dc.date.accessioned
2021-08-23T23:11:39Z
Available date
dc.date.available
2021-08-23T23:11:39Z
Publication date
dc.date.issued
2020
Cita de ítem
dc.identifier.citation
ACS Omega 2020, 5, 29477−29491
es_ES
Identifier
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10.1021/acsomega.0c04420
Identifier
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https://repositorio.uchile.cl/handle/2250/181421
Abstract
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Characterization and control of surfaces and interfaces are critical for photovoltaic and photocatalytic applications. In
this work, we propose CH3NH3PbI3 (MAPI) perovskite slab models whose energy levels, free of quantum confinement, explicitly
consider the spin−orbit coupling and thermal motion. We detail methodological tools based on the density functional theory that
allow achieving these models at an affordable computational cost, and analytical corrections are proposed to correct these effects in
other systems. The electronic state energies with respect to the vacuum of the static MAPI surface models, terminated in PbI2 and
MAI atomic layers, are in agreement with the experimental data. The PbI2-terminated slab has in-gap surface states, which are
independent of the thickness of the slab and also of the orientation of the cation on the surface. The surface states are not useful for
alignments in photovoltaic devices, while they could be useful for photocatalytic reactions. The energy levels calculated for the MAIterminated
surface coincide with the widely used values to estimate the MAPI alignment with the charge transport materials, i.e.,
−5.4 and −3.9 eV for valence band maximum and conduction band minimum, respectively. Our study offers these slab models to
provide guidelines for optimal interface engineering.
es_ES
Patrocinador
dc.description.sponsorship
1171807
11180984
supercomputing infrastructure of the NLHPC ECM-02
Ministerio de Economia y Competitividad through the project SEHTOP-QC ENE2016-77798-C4-4-R
Millennium Nucleus MultiMat, Chile