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Anisotropic exchange-splitting in semiconductor quantum dots (QDs) results inbright-exciton fine-structure-splitting (FSS) important for quantum informationprocessing. Direct measurement of FSS usually requires single/few QDs atliquid-helium temperatures, because of its sensitivity to QD size and shape,whereas measuring and controlling FSS at an ensemble-level seem to beimpossible unless all the dots are made to be nearly the same. Here we reportstrong bright-exciton FSS up to 1.6 meV in solution-processed CsPbI3 perovskiteQDs, manifested as quantum beats in ensemble-level transient absorption atliquid-nitrogen to room temperatures. The splitting is robust to QD size andshape heterogeneity, and increases with decreasing temperature, pointingtowards a mechanism associated with orthorhombic distortion of perovskitelattice. Effective-mass-approximation calculations reveal an intrinsic"fine-structure gap" that agrees well with the observed FSS. This gap stemsfrom an avoided crossing of bright-excitons confined inorthorhombically-distorted QDs that are bounded by the pseudocubic {100} familyof planes.

Lattice distortion inducing exciton splitting and coherent quantum beating in CsPbI3 perovskite quantum dots