Quasi-2D Ruddlesden-Popper halide perovskites with a large exciton binding energy, self-assembled quantum wells and high quantum yield draw attention for optoelectronic device applications. Thin films of these quasi-2D perovskites consist of a mixture of domains having different dimensionality, allowing energy funneling from lower-dimensional nanosheets (narrower bandgap domains) to three-dimensional nanocrystals (wide bandgap domains). Here, the quality of quasi-2D perovskite (PEA)2(FA)3Pb4Br13 is controlled by solution engineering. Grazing-incidence wide-angle X-ray scattering (GIWAXS) measurements were conducted to study the crystal orientation, and transient absorption spectroscopy (TAS) measurements were conducted to study the charge carrier dynamics. Our data show that the highly oriented 2D crystals have a faster energy transfer to the low bandgap regime (< 0.5 ps) compared to less oriented films. High-performance LEDs can be realized with these 2D films. Finally, amplified spontaneous emission is achieved with an ultralow threshold of 4.16 μJ/cm2 and distributed feedback lasers are realized.
Our results show that it is important to control the morphology and spatial domain distribution of the quasi-2D films to achieve efficient energy transfer, which is a critical requirement for optoelectronic devices.