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Electronic Structure of Two-Dimensional Lead(II) Iodide Perovskites: An Experimental and Theoretical Study
Uppsala Univ, Dept Phys & Astron, Solid State Phys, Angstrom Lab, Box 516, SE-75121 Uppsala, Sweden..
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.ORCID iD: 0000-0002-0387-2993‚Äč
Uppsala Univ, Dept Engn Sci, Solid State Phys, Angstrom Lab, SE-75121 Uppsala, Sweden..
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Applied Material Physics. KTH, School of Chemical Science and Engineering (CHE), Centres, Centre of Molecular Devices, CMD.ORCID iD: 0000-0001-5069-3245
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2018 (English)In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 30, no 15, p. 4959-4967Article in journal (Refereed) Published
Abstract [en]

Layered two-dimensional (2D) hybrid organic-inorganic perovskites (HOP) are promising materials for light-harvesting applications because of their chemical stability, wide flexibility in composition and dimensionality, and increases in photovoltaic power conversion efficiencies. Three 2D lead iodide perovskites were studied through various X-ray spectroscopic techniques to derive detailed electronic structures and band energetics profiles at a titania interface. Core-level and valence band photoelectron spectra of HOP were analyzed to resolve the electronic structure changes due to the reduced dimensionality of inorganic layers. The results show orbital narrowing when comparing the HOP, the layered precursor PbI2, and the conventional 3D (CH3NH3)PbI3 such that different localizations of band edge states and narrow band states are unambiguously due to the decrease in dimensionality of the layered HOPs. Support from density functional theory calculations provide further details on the interaction and band gap variations of the electronic structure. We observed an interlayer distance dependent dispersion in the near band edge electronic states. The results show how tuning the interlayer distance between the inorganic layers affects the electronic properties and provides important design principles for control of the interlayer charge transport properties, such as the change in effective charge masses as a function of the organic cation length. The results of these findings can be used to tune layered materials for optimal functionality and new applications.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2018. Vol. 30, no 15, p. 4959-4967
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Condensed Matter Physics
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URN: urn:nbn:se:kth:diva-234611DOI: 10.1021/acs.chemmater.8b00909ISI: 000442186500014Scopus ID: 2-s2.0-85050821628OAI: oai:DiVA.org:kth-234611DiVA, id: diva2:1248177
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QC 20180914

Available from: 2018-09-14 Created: 2018-09-14 Last updated: 2018-09-14Bibliographically approved

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Safdari, MajidLiu, PengKloo, LarsGardner, James M.

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