Exploring the potential of Sn–Ge based hybrid organic–inorganic perovskites: A density functional theory based computational screening study

Hybrid organic-inorganic perovskite solar cells have attracted significant attention in the field of optoelectronics due to their exceptional photovoltaic and optoelectronic properties. Although lead (Pb)-based perovskites exhibit the highest power conversion efficiencies, concerns about their toxicity and environmental impact have prompted significant research activities to explore alternative compositions. In this regard, a special emphasis has been devoted to tin (Sn) and germanium (Ge) based perovskites. In order to reveal the full potential of Sn-Ge based perovskites, we computationally screened perovskites with a general formula of A0.5A0.5'SnyGe1-yX3 (y = 0.00, 0.25, 0.50, 0.75, 1.00) at the density functional theory level, particularly using the HSE06 hybrid functional. By using 18 A/A'-cations, four X-anions, and five different y compositions, a total of 7695 perovskites in cubic (C), orthogonal (O), and tetragonal (T) phases were considered, and the most promising ones have been filtered out based on their formation energy and bandgap. More specifically, 596, 525, and 542 C-, O-, and T-phase perovskites have been identified with a HSE06 bandgap range of 1.0-2.0 eV. While the Sn1.00Ge0.00 composition was dominated for both C- and O-phases, for the T-phase, a higher number of promising perovskites were obtained with the Sn0.75Ge0.25 composition. It has also been found that Sn-rich perovskites exhibit more favorable bandgap characteristics compared to Ge-rich ones. FA, MS, MA, K, Cs, and Rb are the most favored A/A'-cations in these promising perovskites. Moreover, I- overwhelmingly prevails as the dominant anion. Further experimental validation may uncover the true capabilities and practical applicability of these promising perovskites.