Carrier Dynamics Engineering for High-Performance Electron-Transport-Layer-free Perovskite Photovoltaics

Electron-transport-layer-free (ETL-free) device architectures are promising designs for perovskite photovoltaics because they offer simpler configurations, low cost, and convenience for versatile optoelectronics. However, the development of ETL-free photovoltaics is hindered by their low performance. Herein, we reveal that a low electron-injection rate at the ETL-free interface is responsible for the performance loss. Moreover, we demonstrate that improving carrier lifetimes in the perovskite films can remedy the poor carrier extraction at interfaces, enabling carrier collection efficiency in ETL-free photovoltaics to approach that in ETL-containing devices. Using perovskite films with microsecond carrier lifetimes, we obtained ETL-free devices with a power conversion efficiency (PCE) of 19.5%, nearly eliminated hysteresis, and good stability. Such a PCE value is comparable to that (20.7%) of the analogous ETL-containing photovoltaics. These results offer opportunities for ETL-free architecture designs in the perovskite photovoltaics family. More importantly, this research provides a general approach to improving the performance of photovoltaics with low-injection-rate interfaces.