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Towards increasing the stability of perovskite solar cells, the addition of Cs<sup>+</sup> is found to be a rational approach. Recently triple cation based perovskite solar cells were found to be more effective in terms of stability and efficiency. Heretofore they were unexplored, so we probed the Cs/MA/FA (cesium/methyl ammonium/formamidinium) cation based perovskites by X-ray photoelectron spectroscopy (XPS) and correlated their compositional features with their solar cell performances. The Cs<sup>+</sup> content was found to be optimum at 5%, when incorporated in the (MA<sub>0.15</sub>FA<sub>0.85</sub>)Pb(I<sub>0.85</sub>Br<sub>0.15</sub>)<sub>3</sub> lattice, because the corresponding device yielded the highest fill factor compared to the perovskite without Cs<sup>+</sup> and with 10% Cs<sup>+</sup>. XPS studies distinctly reveal how Cs<sup>+</sup> aids in maintaining the expected stoichiometric ratios of I : Pb<sup>2+</sup>, I : N and Br : Pb<sup>2+</sup> in the perovskites, and how the valence band (VB) edge is dependent on the Cs<sup>+</sup> proportion, which in turn governs the open circuit voltage. Even at a low content of 5%, Cs<sup>+</sup> resides deep within the absorber layer, and ensures minimum distortion of the VB level (compared to 0% and 10% Cs<sup>+</sup> perovskites) upon Ar<sup>+</sup> sputtering, thus allowing the formation of a stable robust material that delivers excellent solar cell response. This study which brings out the role of Cs<sup>+</sup> is anticipated to be of paramount significance to further engineer the composition and improve device performances.
Published in: Physical Chemistry Chemical Physics
Volume 19, Issue 5, pp. 4069-4077
DOI: 10.1039/c6cp08022g