Journal
ACS ENERGY LETTERS
Volume 5, Issue 2, Pages 347-352Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.9b02490
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Funding
- Center for Hybrid Organic Inorganic Semiconductors for Energy (CHOISE), an Energy Frontier Research Center - Office of Basic Energy Sciences, Office of Science within the U.S. Department of Energy [DE-AC36-08GO28308]
- NREL
- Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
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Hybrid organic-inorganic lead halide perovskites have shown promising results as active layers in light-emitting diodes, typically utilizing the near-monochromatic, free exciton emission. Some perovskite compounds, however, show broad-band emission that is more intense than the free exciton counterpart. In this study, we show that the light emission properties of ? Ruddlesden-Popper hybrid perovskites PEA(2)MA(n-1)Pb(n)I(3n+1) (PEA = phenethylammonium, MA = methylammonium) can be tuned by Sn alloying and are highly sensitive to Sn %. With increasing dimensionality, the broad-band emission quantum yield decreases drastically, from 23% in n = 1 to <1% for the n = 3 compound. Using density functional theory calculations and transient reflectance spectroscopy, the broad emission is identified as originating from self-trapped excitons. A dynamic picture of the formation process is also presented, for which ultrafast (<5 ps) hole-trapping at the Sn site is the first step, followed by electron localization from Coulombic interaction. These findings are especially valuable for designing perovskite materials with intense room-temperature broad-band emission for solid-state lighting applications.
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