Computational Study of Dipole Radiation in Re-Absorbing Perovskite Semiconductors for Optoelectronics.

Compared to organic emitters, perovskite materials generally have a small Stokes shift and correspondingly large re-absorption of dipole emission. Classical optical modelling methods ignoring re-absorption do not provide an adequate description of the observed light emission properties. Here, optical modelling methods and design rules for perovskite light-emitting diodes are presented. The transfer-matrix formalism is used to quantify the Poynting vectors generated by a dipole radiating inside a perovskite optoelectronic device. A strategy is presented to deal with non-radiative coupling to nearby emissive material that can otherwise lead to non-physical divergence in the calculation. Stability issues are also investigated regarding coherence of the light propagating in the substrate and the absence of a light absorber in the system. The benefit of the photon recycling effect is taken into account by recursive calculation of the dipole generation profile. The simulation results predict that a high external quantum efficiency of ≈40% is achievable in formamidinium lead triiodide-based perovskite light-emitting diodes, by optimization of microcavity, dipole orientation, and photon recycling effects. Contrary to conventional device structures currently reported, this work highlights the benefits of thick charge transport layers and thick perovskite with small Stokes shift.