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Issue 23, 2019
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On the absence of a phonon bottleneck in strongly confined CsPbBr3 perovskite nanocrystals

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Abstract

In traditional solar cells, photogenerated energetic carriers (so-called hot carriers) rapidly relax to band edges via emission of phonons, prohibiting the extraction of their excess energy above the band gap. Quantum confined semiconductor nanocrystals, or quantum dots (QDs), were predicted to have long-lived hot carriers enabled by a phonon bottleneck, i.e., the large inter-level spacings in QDs should result in inefficient phonon emissions. Here we study the effect of quantum confinement on hot carrier/exciton lifetime in lead halide perovskite nanocrystals. We synthesized a series of strongly confined CsPbBr3 nanocrystals with edge lengths down to 2.6 nm, the smallest reported to date, and studied their hot exciton relaxation using ultrafast spectroscopy. We observed sub-ps hot exciton lifetimes in all the samples with edge lengths within 2.6–6.2 nm and thus the absence of a phonon bottleneck. Their well-resolved excitonic peaks allowed us to quantify hot carrier/exciton energy loss rates which increased with decreasing NC sizes. This behavior can be well reproduced by a nonadiabatic transition mechanism between excitonic states induced by coupling to surface ligands.

Graphical abstract: On the absence of a phonon bottleneck in strongly confined CsPbBr3 perovskite nanocrystals

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Supplementary files

Article information


Submitted
19 Mar 2019
Accepted
05 May 2019
First published
06 May 2019

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2019,10, 5983-5989
Article type
Edge Article

On the absence of a phonon bottleneck in strongly confined CsPbBr3 perovskite nanocrystals

Y. Li, R. Lai, X. Luo, X. Liu, T. Ding, X. Lu and K. Wu, Chem. Sci., 2019, 10, 5983
DOI: 10.1039/C9SC01339C

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