Band-edge Exciton Fine Structure and Exciton Recombination Dynamics in Single crystals of Layered Hybrid Perovskites

Abstract: Two-dimensional (2D) perovskite materials have recently re-attracted intense research interest for applications in photovoltaics and optoelectronics. As a consequence of the dielectric and quantum confinement effect, they show strongly bound and stable excitons at room temperature. In this report, the band-edge exciton fine structure and in particular its exciton and biexciton dynamics in high quality crystals of (PEA)2PbI4 are investigated. A comparison of bulk and surface exciton lifetimes yields a room temperature surface recombination velocity of 2x10^3cm/s and an intrinsic lifetime of 185ns. Biexciton emission is evidenced at room temperature, with binding energy of about 45meV and a lifetime of 80ps. At low temperature, exciton state splitting is observed, which is caused by the electron-hole exchange interaction. Transient photoluminescence resolves the low-lying dark exciton state, with a bright/dark splitting energy estimated to be 10meV. This work contributes to understand the complex scenario of the elementary photoexcitations in 2D perovskites.