Photoemission of the Upconverted Hot Electrons in Mn-Doped CsPbBr3 Nanocrystals

Hot electrons play a crucial role in enhancing the efficiency of photon-to-current conversion or photocatalytic reactions. In semiconductor nanocrystals, energetic hot electrons capable of photoemission can be generated via the upconversion process involving the dopant-originated intermediate state, currently known only in Mn-doped cadmium chalcogenide quantum dots. Here, we report that Mn-doped CsPbBr3 nanocrystals are an excellent platform for generating hot electrons via upconversion that can benefit from various desirable exciton properties and the structural diversity of metal halide perovskites (MHP). 2-dimensional Mn-doped CsPbBr$_3$ nanoplatelets are particularly advantageous for hot electron upconversion due to the strong exciton-dopant interaction mediating the upconversion process. Furthermore, nanoplatelets reveal evidence for the hot electron upconversion via long-lived dark exciton in addition to bright exciton that may enhance the upconversion efficiency. This study not only establishes the feasibility of hot electron upconversion in MHP host but also demonstrates the potential merits of 2-dimensional MHP nanocrystals in hot electron upconversion.