Minimizing and Controlling Hydrogen for Highly Efficient Formamidinium Lead Triiodide Solar Cells

Formamidinium lead triiodide (FAPbI(3)) currently holds the record conversion efficiency in the single-junction perovskite solar cell. Iodine management is known to be essential to suppress defect-induced nonradiative losses in FAPbI(3) active layers. However, the origin of nonradiative losses and the underlying mechanism of suppressing such losses by iodine-concentration management remain unknown. Here, through first-principles simulation, we demonstrate that native point defects are not responsible for the nonradiative losses in FAPbI(3). Instead, hydrogen ions, which can be abundant under both iodine-rich and iodine-poor conditions in FAPbI(3), act as efficient nonradiative recombination centers and are proposed to be responsible for the suppressed power conversion efficiency. Moreover, iodine-moderate synthesis conditions can favor the formation of electrically inactive molecular hydrogen, which can dramatically suppress the detrimental hydrogen ions. This work identifies the dominant nonradiative recombination centers in the widely used FAPbI(3) layers and rationalizes how the prevailing iodine management reduces the nonradiative losses. Minimizing the unintentional hydrogen incorporation in the perovskite is critical for achieving high device performance.

Automated summary

This study reveals that hydrogen ions, rather than native point defects, act as the dominant nonradiative recombination centers in FAPbI(3) perovskite solar cells. It also suggests that moderate iodine synthesis conditions can suppress the formation of harmful hydrogen ions and improve device performance.