Journal article
High Chloride Doping Levels Stabilize the Perovskite Phase of Cesium Lead Iodide
Nano letters, v 16(6), pp 3563-3570
01 Jun 2016
PMID: 27135266
Featured in Collection : UN Sustainable Development Goals @ Drexel
Abstract
Cesium lead iodide possesses an excellent combination of band gap and absorption coefficient for photovoltaic applications in its perovskite phase. However, this is not its equilibrium structure under ambient conditions. In air, at ambient temperature it rapidly transforms to a nonfunctional, so-called yellow phase. Here we show that chloride doping, particularly at levels near the solubility limit for chloride in a cesium lead iodide host, provides a new approach to stabilizing the functional perovskite phase. In order to achieve high doping levels, we first co-deposit colloidal nanocrystals of pure cesium lead chloride and cesium lead iodide, thereby ensuring nanometer-scale mixing even at compositions that potentially exceed the bulk miscibility of the two phases. The resulting nanocrystal solid is subsequently fused into a polycrystalline thin film by chemically induced, room-temperature sintering. Spectroscopy and X-ray diffraction indicate that the chloride is further dispersed during sintering and a polycrystalline mixed phase is formed. Using density functional theory (DFT) methods in conjunction with nudged elastic band techniques, low-energy pathways for interstitial chlorine diffusion into a majority-iodide lattice were identified, consistent with the facile diffusion and fast halide exchange reactions observed. By comparison to DFT-calculated values (with the PBE exchange-correlation functional), the relative change in band gap and the lattice contraction are shown to be consistent with a Cl/I ratio of a few percent in the mixed phase. At these incorporation levels, the half-life of the functional perovskite phase in a humid atmosphere increases by more than an order of magnitude.
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Details
- Title
- High Chloride Doping Levels Stabilize the Perovskite Phase of Cesium Lead Iodide
- Creators
- Subham Dastidar - Drexel UniversityDavid A. Egger - Weizmann Institute of ScienceLiang Z. Tan - University of PennsylvaniaSamuel B. Cromer - Drexel UniversityAndrew D. Dillon - Drexel UniversityShi Liu - Carnegie Institution for ScienceLeeor Kronik - Weizmann Institute of ScienceAndrew M. Rappe - University of PennsylvaniaAaron T. Fafarman - Drexel University
- Publication Details
- Nano letters, v 16(6), pp 3563-3570
- Publisher
- American Chemical Society; Washington, DC
- Number of pages
- 8
- Grant note
- J3608-N20 / Austrian Science Fund (FWF) Carnegie Institution for Science J 3608 / Austrian Science Fund (FWF) Dana and Yossie Hollander Lise Meitner Minerva Center for Computational Chemistry N00014-14-1-0761 / Office of Naval Research DE-FG02-07ER46431 / Department of Energy Office of Basic Energy Sciences; United States Department of Energy (DOE) Drexel University
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Chemical and Biological Engineering
- Web of Science ID
- WOS:000377642700023
- Scopus ID
- 2-s2.0-84974806673
- Other Identifier
- 991019168753304721
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- Collaboration types
- Domestic collaboration
- International collaboration
- Web of Science research areas
- Chemistry, Multidisciplinary
- Chemistry, Physical
- Materials Science, Multidisciplinary
- Nanoscience & Nanotechnology
- Physics, Applied
- Physics, Condensed Matter