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https://doi.org/10.21203/rs.3....
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Observation of an Ultrafast Exciton Transport Regime at Early Times in Quantum Dot Solids

Authors: Zhang, Zhilong; Sung, Jooyoung; Toolan, Daniel; Han, Sanyang; Weir, Michael; Xiao, James; Dowland, Simon; +5 Authors

Observation of an Ultrafast Exciton Transport Regime at Early Times in Quantum Dot Solids

Abstract

Abstract Understanding and engineering exciton transport in quantum dot (QD) solids is both of fundamental interest and crucial to their broad applications in devices1-6. Till date, studies of exciton transport in QD solids on pico/nano-second timescales have led to the conclusion that closer packing of QDs enables faster exciton transport, while energetic/structural heterogeneity leads to reduction of exciton diffusivity over time7,8. Here we study PbS QD solids using transient absorption microscopy with 13 femtoseconds time resolution and 10 nm spatial precision. We find exciton diffusivities in the range of ~102 cm2 s-1 within the first few hundred femtoseconds after photoexcitation, followed by the transition to a slower transport regime with diffusivities in the range 10-1 to 1 cm2 s-1. Counterintuitively, the initial diffusivity is higher and the time before the transition to the slower transport phase is longer in QD solids with longer ligand lengths. This suggests a transition from early-time transport of delocalized excitons to later time hopping based transport of localized excitons, where QD packing density and heterogeneity accelerate the localization process. Our results reveal a new regime for exciton transport in QD solids and provide design rules to engineer desired transport properties in these systems on a range of timescales.

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citations
This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Citations provided by BIP!
popularity
This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.
BIP!Popularity provided by BIP!
influence
This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Influence provided by BIP!
impulse
This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.
BIP!Impulse provided by BIP!
0
Average
Average
Average
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