Journal
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 16, Issue 40, Pages 22122-22130Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/C4CP03533J
Keywords
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Funding
- National Renewable Energy Laboratory Director's Fellowship
- U.S. Department of Energy/National Renewable Energy Laboratory's Laboratory Directed Research and Development (LDRD) program
- Division of Chemical Sciences, Geosciences, and Biosciences
- Office of Basic Energy Sciences of the US Department of Energy
- US Department of Energy
- Office of Basic Energy Sciences, Energy Frontier Research Centers [DE-AC36-08GO28308]
- US-India Partnership to Advance Clean Energy Research (PACE-R)
- Solar Energy Research Institute for India and the United States (SERIIUS)
- Government of India, through the Department of Science and Technology [IUSSI4JCERDC-SERIIUS/2012]
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Using X-ray and ultraviolet photoelectron spectroscopy, the surface band positions of solution-processed CH(3)NH(3)Pbl(3) perovskite thin films deposited on an insulating substrate (Al2O3), various n-type (TiO2, ZrO2, ZnO, and F:SnO2 (FTO)) substrates, and various p-type (PEDOT:PSS, NiO, and Cu2O) substrates are studied. Many-body GW calculations of the valence band density of states, with spin orbit interactions included, show a clear correspondence with our experimental spectra and are used to confirm our assignment of the valence band maximum. These surface-sensitive photoelectron spectroscopy measurements result in shifting of the CH(3)NH(3)Pbl(3) valence band position relative to the Fermi energy as a function of substrate type, where the valence band to Fermi energy difference reflects the substrate type (insulating-, n-, or p-type). Specifically, the insulating- and n-type substrates increase the CH(3)NH(3)Pbl(3) valence band to Fermi energy difference to the extent of pinning the conduction band to the Fermi level; whereas, the p-type substrates decrease the valence band to Fermi energy difference. This observation implies that the substrate's properties enable control over the band alignment of CH(3)NH(3)Pbl(3) perovskite thin-film devices, potentially allowing for new device architectures as well as more efficient devices.
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