Journal
NANO LETTERS
Volume 15, Issue 8, Pages 5191-5199Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.5b01430
Keywords
Perovskite; nanocrystals; anion exchange reaction; composition tuning; photodetectors
Categories
Funding
- NRF [20110020090, 2014051259, 2012-R1A1A-2039084]
- Korea University Grant
- Jeonju University
- MOST
- POSTECH
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In recent years, methylammonium lead halide (MAPbX(3), where X = Cl, Br, and I) perovskites have attracted tremendous interest caused by their outstanding photovoltaic performance. Mixed halides have been frequently used as the active layer of solar cells, as a result of their superior physical properties as compared to those of traditionally used pure iodide. Herein, we report a remarkable finding of reversible halide-exchange reactions of MAPbX(3), which facilitates the synthesis of a series of mixed halide perovskites. We synthesized MAPbBr(3) plate-type nanocrystals (NCs) as a starting material by a novel solution reaction using octylamine as the capping ligand. The synthesis of MAPbBr(3-x)Cl(x) and MAPbBr(3-x)I(x) NCs was achieved by the halide exchange reaction of MAPbBr(3) with MACl and MAI, respectively, in an isopropyl alcohol solution, demonstrating full-range band gap tuning over a wide range (1.6-3 eV). Moreover, photodetectors were fabricated using these composition-tuned NCs; a strong correlation was observed between the photocurrent and photoluminescence decay time. Among the two mixed halide perovskite series, those with I-rich composition (x = 2), where a sole tetragonal phase exists without the incorporation of a cubic phase, exhibited the highest photoconversion efficiency. To understand the composition-dependent photoconversion efficiency, first-principles density-functional theory calculations were carried out, which predicted many plausible configurations for cubic and tetragonal phase mixed halides.
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