Proceedings of 6th International Conference on Hybrid and Organic Photovoltaics (HOPV14)
Publication date: 1st March 2014
Solution-processable organic-inorganic hybrid solar cells based on the lead iodide perovskite (CH3NH3PbI3) exhibit remarkably high power conversion efficiency (PCE).The key issue for optimizing PCE is to match the electronic energy levels of the perovskite to the adjacent organic hole and electron transporting layers. Here we employ ab initio calculations and photoelectron spectroscopy to unravel the electronic structure and charge redistribution between organic hole acceptor Spiro-OMeTAD, electron acceptor PCBM and CH3NH3PbI3 with surface orientations (001) or (100). We found that calculated energy levels are in good agreement with experimental values obtained by ultraviolet photoelectron spectroscopy measurements. Compared to the (100) orientation, the CH3NH3PbI3 (001) surface tends to favour hole injection to Spiro-OMeTAD and electron transfer to PCBM, resulting in larger number of transferred Bader charges and hole/electron accumulation at the CH3NH3PbI3/organic interfaces. Molecular dynamic simulations suggest that this is due to the stronger electronic coupling induced by thermal fluctuations at room temperature, overall indicating that perovskite crystallization and surface orientation are extremely important design parameters to optimize charge separation and extraction in hybrid solar cells.