Persistent enhancement of exciton diffusivity in CsPbBr3 nanocrystal solids

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.

doi:10.1126/sciadv.adj2630

Persistent enhancement of exciton diffusivity in CsPbBr₃ nanocrystal solids

Journal Article · Wed Feb 21 00:00:00 EST 2024 · Science Advances

DOI:https://doi.org/10.1126/sciadv.adj2630· OSTI ID:2471952

^[1]; Saris, Seryio ^[2]; ^[3]; ^[3]; ^[3]; Krieg, Franziska ^[4]; ^[4]; Willard, Adam P. ^[3]; ^[3]

Massachusetts Institute of Technology (MIT), Cambridge, MA (United States); OSTI
Massachusetts Institute of Technology (MIT), Cambridge, MA (United States); Ecole Polytechnique Federale Lausanne (EPFL) (Switzerland)
Massachusetts Institute of Technology (MIT), Cambridge, MA (United States)
Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); Swiss Federal Laboratories for Materials Science and Technology (Empa), Dübendorf (Switzerland)

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.

View Accepted Manuscript (DOE)

Research Organization:: Massachusetts Institute of Technology (MIT), Cambridge, MA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019345; SC0019998

OSTI ID:: 2471952

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 8 Vol. 10; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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