Exciton-acoustic phonon coupling revealed by resonant excitation of single perovskite nanocrystals

Single perovskite nanocrystals have attracted great research attention very recently due to their potential quantum-information applications, which critically depend on the development of powerful optical techniques to resolve delicate exciton photophysics. Here we have realized resonant and near-resonant excitations of single perovskite CsPbI(3) nanocrystals, with the scattered laser light contributing to only ~10% of the total collected signals. This allows us to estimate an ultranarrow photoluminescence excitation linewidth of ~11.32 µeV for the emission state of a single CsPbI(3) nanocrystal, corresponding to an exciton dephasing time of ~116.29 ps. Meanwhile, size-quantized acoustic phonons can be resolved from a single CsPbI(3) nanocrystal, whose coupling with the exciton is proposed to arise from the piezoelectric potential. The ability to collect resonance fluorescence from single CsPbI(3) nanocrystals, with the subsequent revelation of exciton-acoustic phonon coupling, has marked a critical step towards their steady advancement into superior quantum-light sources.