Composition-Dependent Optoelectronic Properties of Mixed 2D/3D Metal Halide Perovskite Films for Light-Emitting Diodes

Low-dimensional perovskites with large organic cations have shown great potential for boosting the luminescence efficiency of metal halide perovskite light-emitting diodes (PeLEDs). Although numerous successful results have been obtained for mixed two-dimensional (2D)/three-dimensional (3D) perovskite films, the correlation of the optoelectronic properties with the crystallographic properties and film composition remains elusive. Herein, we investigated the optoelectronic quality of thin films and their impact on luminescence and transport behaviors in a mixed 2D/3D perovskite system containing 2D butylammonium lead bromide (BA2PbBr4) and 3D formamidinium lead bromide (FAPbBr3). Ultrafast transient absorption and temperature-dependent photoluminescence measurements revealed distinct changes in nonemissive decay of the excited states, including the vibrational coupling properties. These behaviors could then be closely correlated with the crystallographic evolution of the perovskite films. We rationalized the performance of PeLED devices and determined the possible limitations to further utilize the advantageous properties of mixed 2D/3D perovskite systems by examining both the luminescence and electrical properties of the perovskite films.