Achieving Up-Conversion Amplified Spontaneous Emission through Spin Alignment between Coherent Light-Emitting Excitons in Perovskite Microstructures

Abstract

Metal hybrid perovskites have presented interesting infrared-to-visible up-conversion light-emitting lasing properties through multi-photon absorption. Here, when the optical pumping switches between circular and linear polarization, up-conversion amplified spontaneous emission (ASE) intensity exhibits large and small amplitudes, respectively, leading to a positive up-conversion ΔASE in the CsPbBr3 perovskite microrods. This observed phenomenon demonstrates that the coherent interaction between coherent light-emitting excitons is indeed established at the up-conversion ASE regime in the CsPbBr3 perovskite microrods. In addition, the positive up-conversion ΔASE indicates the orbital magnetic dipoles between coherent light-emitting excitons are conserved during up-conversion ASE action. Essentially, the up-conversion ΔASE results provide evidence that shows up-conversion ASE can be realized by the orbit−orbit polarization interaction between light-emitting excitons. Moreover, up-conversion ASE proportionally increased as the pumping fluence increased, which shows that orbit–orbit polarization interaction can be gradually enhanced between coherent light-emitting excitons by increasing pumping density in the CsPbBr3 perovskite microrods. Substantially, our studies provide a fundamental understanding of the spin alignment between coherent light-emitting excitons towards developing spin-dependent nonlinear lasing actions in metal halide perovskites.