Persistent enhancement of exciton diffusivity in CsPbBr3 nanocrystal solids
Name
sciadv.adj2630.pdf
Description
Published version
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1.65 MB
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Checksum (MD5)
a009a9faf7716f39fb658495b0d6a809
Author(s)
Shcherbakov-Wu, Wenbi
Saris, Seryio
Sheehan, Thomas John
Wong, Narumi Nagaya
Powers, Eric R
Krieg, Franziska
Kovalenko, Maksym V
Willard, Adam P
Tisdale, William A
Date Issued
February 21, 2024
Journal
Science Advances
Publisher
American Association for the Advancement of Science
Citation
Wenbi Shcherbakov-Wu et al. ,Persistent enhancement of exciton diffusivity in CsPbBr3 nanocrystal solids.Sci. Adv.10, eadj2630 (2024).
Version
Final published version
Abstract
In semiconductors, exciton or charge carrier diffusivity is typically described as an inherent material property. Here, we show that the transport of excitons among CsPbBr3 perovskite nanocrystals (NCs) depends markedly on how recently those NCs were occupied by a previous exciton. Using transient photoluminescence microscopy, we observe a striking dependence of the apparent exciton diffusivity on excitation laser power that does not arise from nonlinear exciton-exciton interactions or thermal heating. We interpret our observations with a model in which excitons cause NCs to transition to a long-lived metastable configuration that markedly increases exciton transport. The exciton diffusivity observed here (>0.15 square centimeters per second) is considerably higher than that observed in other NC systems, revealing unusually strong excitonic coupling between NCs. The finding of a persistent enhancement in excitonic coupling may help explain other photophysical behaviors observed in CsPbBr3 NCs, such as superfluorescence, and inform the design of optoelectronic devices.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
Massachusetts Institute of Technology. Department of Chemistry
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DOI of Published Version
10.1126/sciadv.adj2630
