Journal
ADVANCED OPTICAL MATERIALS
Volume 5, Issue 9, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adom.201700139
Keywords
CH3NH3PbI3 single crystals; mixed halide perovskite (CH3NH3PbI3-xClx) films; surface band bending; X-ray and ultraviolet photoelectron spectroscopy
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Funding
- Helmholtz Energy Alliance Hybrid Photovoltaics
- Joint Graduate School HyPerCells of the University of Potsdam
- Helmholtz Zentrum Berlin
- DFG [Sfb951]
- NSFC Research Fund for International Young Scientists [11550110176]
- Soochow University-Western University Center for Synchrotron Radiation Research
- Collaborative Innovation Center of Suzhou Nano Science and Technology (NANO-CIC)
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This study investigates the effect of white light illumination on the electronic and chemical properties of mixed halide perovskite (CH3NH3PbI3-xClx) thin films and CH3NH3PbI3 single crystals using photoelectron and absorption spectroscopy. The pristine materials' surfaces are found to be n-type because of surface band bending due to the presence of donor levels, likely consisting of reduced lead (Pb-0) that acts as surface traps. When illuminating the sample with white light (up to 1 sun), the valence features shifted to lower binding energy due to surface photovoltage, i.e., the bulk of the materials is much less n-type. However, the surface photovoltage is only partially reversible and vanishes for prolonged illumination time. Concomitantly, a high concentration of metallic Pb-0 is found, which induces strong Fermi-level pinning and quenching of the surface photovoltage. This is accompanied also by the formation of PbI2 defects. Similar experiments on single crystals reveal the presence of a high concentration of reduced (metallic) Pb-0 at the sample surface after cleaving. The present findings indicate that the chemical and electronic properties of perovskite films are very sensitive to white light illumination. Accounting for these light-induced material changes is important to fully understand its photophysical properties and for improving the lifetime of perovskite-based devices.
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