Closed-shell light-emitting diodes (LEDs) suffer from the internal quantum efficiency (IQE) limitation imposed by optically inactive triplet excitons. Here we show an undiscovered emission mechanism of lead-halide-perovskites (LHPs) APbX3 (A=Cs/CN2H5; X=Cl/Br/I) that circumvents the efficiency limit of closed-shell LEDs. Though efficient emission is prohibited by optically inactive J=0 in inversion symmetric LHPs, the anharmonicity arising from stereochemistry of Pb and resonant orbital-bonding network along the imaginary A+⋯X− (T1u) transverse optical (TO) modes, breaks the inversion symmetry and introduces disorder and Rashba-Dresselhaus spin-orbit coupling (RD-SOC). This leads to bright co-helical and dark anti-helical excitons. Many-body theory and first-principles calculations affirm that the optically active co-helical exciton is the lowest excited state in organic/inorganic LHPs. Thus, RD-SOC can drive to achieve the ideal 50 % IQE by utilizing anharmonicity, much over the 25 % IQE limitation for closed-shell LEDs.
Cite
@article{arxiv.2004.02329,
title = {Anharmonicity-driven Rashba co-helical excitons break quantum efficiency limitation},
author = {Chang Woo Myung and Kwang S. Kim},
journal= {arXiv preprint arXiv:2004.02329},
year = {2020}
}