Journal
ACS ENERGY LETTERS
Volume 1, Issue 2, Pages 360-366Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.6b00196
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Funding
- U.S. Department of Energy Office of Energy Efficiency and Renewable Energy [DE-AC36-08-GO28308]
- Hybrid Perovskite Solar Cell program of the National Center for Photovoltaics - U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Solar Energy Technologies Office
- DOE-EERE program at NREL [25786]
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Photovoltaic applications of perovskite semiconductor material systems have generated considerable interest in part because of predictions that primary defect energy levels reside outside the bandgap. We present experimental evidence that this enabling material property is present in the halide-lead perovskite, CH3NH3PbI3 (MAPbI(3)), consistent with theoretical predictions. By performing X-ray photoemission spectroscopy, we induce and track dynamic chemical and electronic transformations in the perovskite. These data show compositional changes that begin immediately with exposure to X-ray irradiation, whereas the predominant electronic structure of the thin film on compact TiO2 appears tolerant to the formation of compensating defect pairs of V-I and V-MA and for a large range of I/Pb ratios. Changing film composition is correlated with a shift of the valence-band maximum only as the halide-lead ratio drops below 2.5. This delay is attributed to the invariance of MAPbI(3) electronic structure to distributed defects that can significantly transform the electronic density of states only when in high concentrations.
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