Perovskite solar cells (PSCs) are being developed rapidly and exhibit greatly potential commercialization. Herein, it is found that the device performance can be improved by manipulating the migration of iodine ions via reverse-biasing, for example, at -0.4 V for 3 min in dark. Characterizations suggest that reverse bias can increase the charge recombination resistance, improve carrier transport, and enhance built-in electric field. Iodine ions including iodine interstitials in perovskites are confirmed to migrate and accumulate at the SnO2 /perovskite interface under reverse-basing, which fill iodine vacancies at the interface and interact with SnO2 . First-principles calculations suggest that the SnO2 /perovskite interface with less iodine vacancies has a stronger interaction and higher charge transfer, leading to larger built-in electric field and improved charge transport. Iodine ions that may pass through the SnO2 /perovskite interface are also confirmed to be able to interact with Sn4+ and passivate oxygen vacancies on the surface of SnO2 . Consequently, an efficiency of 23.48% with the open-circuit voltage (Voc ) of 1.16 V is achieved for PSCs with reverse-biasing, as compared with the initial efficiency of 22.13% with a Voc of 1.10 V. These results are of great significance to reveal the physics mechanism of PSCs under electric field.
Keywords: ion migration; perovskite solar cells; reverse bias; vacancy.
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