Quantum beats of exciton-polarons in CsPbI3 perovskite nanocrystals

Abstract

The optical response of semiconductors is governed by coupled electronic and vibrational excitations. In lead-halide perovskite nanocrystals, strong exciton–phonon interaction forms a ladder of exciton-polaron states accessible by femtosecond laser pulses. We demonstrate a fully coherent regime of exciton-polaron dynamics with long optical coherence times (T2 ≈ 300 ps) in CsPbI3 nanocrystals embedded in glass. Using transient two-pulse photon echo at a temperature of 2 K, we observe quantum beats between exciton-polaron states, with decay determined by optical phonon lifetimes of 5-15 ps. Within a four-level model, we directly quantify the exciton–phonon coupling strength through Huang–Rhys factors of 0.05 − 0.12 and 0.02 − 0.04 for low-energy optical phonons with energies of 3.2 and 5.1 meV, respectively. The pronounced size dependence of both coupling strengths and phonon lifetimes offers a route to tune the optical transitions between exciton-polaron states and tailor the coherent optical dynamics in perovskite semiconductors for solid-state quantum technologies.