Long-Lived Exciton Coherence in Mixed-Halide Perovskite Crystals

Nano Lett. 2023 Aug 23;23(16):7397-7403. doi: 10.1021/acs.nanolett.3c01817. Epub 2023 Aug 7.

Abstract

Compositional engineering of the optical properties of hybrid organic-inorganic lead halide perovskites is crucial for the realization of efficient solar cells and light-emitting devices. We study the effect of band gap fluctuations on coherent exciton dynamics in a mixed FA0.9Cs0.1PbI2.8Br0.2 perovskite crystal by using photon echo spectroscopy. We reveal a narrow homogeneous exciton line width of 16 μeV at a temperature of 1.5 K. The corresponding exciton coherence time T2 = 83 ps is exceptionally long due to the localization of excitons at the scale of tens to hundreds of nanometers. From spectral and temperature dependences of the two- and three-pulse photon echo decay, we conclude that for low-energy excitons pure decoherence associated with elastic scattering on phonons is comparable with the exciton lifetime, while for excitons with higher energies, inelastic scattering to lower energy states via phonon emission dominates.

Keywords: FAPbI3; Photon echo; T2; exciton coherence time; four-wave mixing; lead halide perovskite semiconductor.