Bulk Heterojunction Quasi-Two-Dimensional Perovskite Solar Cell with 1.18 V High Photovoltage

Multicomponent quasi-two-dimensional perovskites (Q-2DPs) have efficient luminescence and improved stability, which are highly desirable for light-emitting diode and perovskite solar cell (PSC). However, the lack of radiative recombination at room temperature is still not well understood and the performance of PSC is not good enough as well. The open-circuit voltage ( V_OC) is even lower than that of three-dimensional (3D) PSC with a narrower band gap. In this work, we study the energy transfer of excitons between their multiple components by time-resolved photoluminescence and find that charge transfer from high-energy states to low-energy state is gradually suppressed during elevating temperature owing to trap-mediated recombination. This may reveal the bottleneck of luminescence at room temperature in Q-2DPs, leading to large photovoltage loss in 2D PSC. Therefore, we develop a p-i-n bulk heterojunction (BHJ) structure to reduce the nonradiative recombination and obtain high V_OC of 1.18 V for (PMA)₂MA₄Pb₅I₁₅Cl (33.3% PMA) BHJ device, much higher than that of the planar counterparts. The enhanced efficiency is attributed to the improved exciton dissociation via BHJ interface. Our results provide an important step toward high V_OC and stable 2D PSCs, which could be used for tandem solar cell and colorful photovoltaic windows.