Two-photon excited photoluminescence of single perovskite nanocrystals

Lead-halide perovskite nanocrystals (NCs) have emerged as a novel type of semiconductor nanostructure, attracting great research interests in both fundamental science and practical applications. Here, we compare the optical properties of single CsPbI₃ NCs under both one-photon and two-photon excitations, mainly including the photoluminescence (PL) blinking and PL decay dynamics. By means of the PL saturation effect caused by multi-exciton Auger recombination, we have also estimated a two-photon absorption cross section of ∼6.8 × 10⁶ GM for single CsPbI₃ NCs. The ability to realize efficient two-photon excitation of single perovskite NCs with strongly suppressed background fluorescence will help not only to promote their bio-imaging and biolabeling applications but also to reveal and manipulate their delicate electronic structures for potential usage in quantum information processing.