Tin Halide Perovskite Solar Cells with Open-Circuit Voltages Approaching the Shockley-Queisser Limit

The power conversion efficiency of tin-based halide perovskite solar cells is limited by large photovoltage losses arising from the significant energy-level offset between the perovskite and the conventional electron transport material, fullerene C₆₀. The fullerene derivative indene-C₆₀ bisadduct (ICBA) is a promising alternative to mitigate this drawback, owing to its superior energy level matching with most tin-based perovskites. However, the less finely controlled energy disorder of the ICBA films leads to the extension of its band tails that limits the photovoltage of the resultant devices and reduces the power conversion efficiency. Herein, we fabricate ICBA films with improved morphology and electrical properties by optimizing the choice of solvent and the annealing temperature. Energy disorder in the ICBA films is substantially reduced, as evidenced by the 22 meV smaller width of the electronic density of states. The resulting solar cells show open-circuit voltages of up to 1.01 V, one of the highest values reported so far for tin-based devices. Combined with surface passivation, this strategy enabled solar cells with efficiencies of up to 11.57%. Our work highlights the importance of controlling the properties of the electron transport material toward the development of efficient lead-free perovskite solar cells and demonstrates the potential of solvent engineering for efficient device processing.