Steering perovskite precursor solutions for multijunction photovoltaics

Abstract

Multijunction photovoltaics (PVs) are gaining prominence owing to their superior capability of achieving power conversion efficiencies (PCEs) beyond the radiative limit of single-junction cells, for which improving narrow-bandgap (NBG) tin-lead perovskites is critical for thin-film devices. Here, with a focus on understanding the chemistry of tin-lead perovskite precursor solutions, we find that Sn(ii) species dominate interactions with precursors and additives and uncover the exclusive role of carboxylic acid in regulating solution colloidal properties and film crystallization and ammonium in improving film optoelectronic properties. Materials that combine these two functional groups, amino acid salts, considerably improve the semiconducting quality and homogeneity of perovskite films, surpassing the effect of the individual functional groups when introduced as part of separate molecules. Our enhanced tin-lead perovskite layer allows us to fabricate solar cells with PCEs of 23.9%, 29.7% (certified 29.26%) and 28.7% for single-junction, double-junction and triple-junction devices, respectively. Our 1-cm2 triple-junction devices show PCEs of 28.4% (certified 27.28%). Encapsulated triple-junction cells maintain 80% of their initial efficiencies after 860 h maximum power point tracking (MPPT) in ambient. We further fabricate quadruple-junction devices and obtain PCEs of 27.9% with the highest open-circuit voltage of 4.94 V. This work establishes a new benchmark for multijunction PVs.