Publication date: 1st July 2014
Perovskite light-harvesters have rapidly emerged to the forefront of photovoltaics research exhibiting high power-conversion efficiencies and the promise of low-cost fabrication in devices. Despite recent progress in describing the internal mechanisms for photocurrent generation in perovskite solar cells, a full understanding of the device operation still requires an optical analysis of the device stack. This provides an additional platform for maximising the power-conversion efficiency through a precise determination of parasitic losses caused by optical coherence and absorption in non-photoactive layers. Here we present a transfer-matrix model for the charge-generation profile under sunlight in state-of-the-art perovskite-based planar-heterojunction solar cells using experimental refractive index data from spectroscopic ellipsometry. Excellent agreement between the model and experiment is obtained and reveals some important features of the device operation. In particular, we find the optimum thickness for photocurrent generation, an accurate derivation of the wavelength dependence of the internal quantum efficiency from the external quantum efficiency, and the dependence of the photocurrent on incidence angle. In the latter case, we find that perovskite-based solar cells can compete favourably with conventional technologies not only under AM1.5 illumination but also throughout the day in real-world applications. This work provides important insights into device optimisation which should lead to further improvements in device efficiency.
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