Designing Efficient Energy Funneling Kinetics in Ruddlesden-Popper Perovskites for High-Performance Light-Emitting Diodes

Mixed Ruddlesden-Popper (RP) perovskites are of great interest in light-emitting diodes (LEDs), due to the efficient energy transfer (funneling) from high-bandgap (donor) domains to low-bandgap (acceptor) domains, which leads to enhanced photoluminescence (PL) intensity, long PL lifetime, and high-efficiency LEDs. However, the influence of reduced effective emitter centers in the active emissive film, as well as the implications of electrical injection into the larger bandgap donor material, have not been addressed in the context of an active device. The electrical and optical signatures of the energy cascading mechanisms are critically assessed and modulated in a model RP perovskite series ((C8H17NH3)(2)(CH(NH2)(2))(m-1)PbmBr3m+1). Optimized devices demonstrate a current efficiency of 22.9 cd A(-1) and 5% external quantum efficiency, more than five times higher than systems where funneling is absent. The signature of nonideal funneling in RP perovskites is revealed by the appearance of donor electroluminescence from the device, followed by a reduction in the LED performance