CsPbBr
3 nanocrystals (NCs) encapsulated in a transparent polystyrene (PS) fiber matrix (CsPbBr
3@PS) have been synthesized to protect the NCs. The ultrafast charge delocalization dynamics of the embedded NCs have been demonstrated, and the results are compared with the pristine CsPbBr
3 in toluene. The electrospinning method was employed for the preparation of CsPbBr
3@PS fibers by using a polystyrene solution doped with pre-synthesized CsPbBr
3 and characterized by XRD, HRTEM, and X-ray photoelectron spectroscopy (XPS). Energy level diagrams of CsPbBr
3 and PS suggest that CsPbBr
3@PS fibers make a type I core–shell structure. The carrier cooling for CsPbBr
3@PS fibers is found to be much slower than pure CsPbBr
3 NCs. This observation suggests that photoexcited electrons from CsPbBr
3 NCs get delocalized from the conduction band of the perovskite to lowest unoccupied molecular orbital (LUMO) of the PS fiber matrix. The CsPbBr
3@PS fibers possess remarkable stability under ambient conditions as well as in water over months. The clear understanding of charge carrier relaxation dynamics of CsPbBr
3 confined in PS fibers could help to design robust optoelectronic devices.
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