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

Chemical Science
Yulu LiKaifeng Wu

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.

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Mar 1, 2019·Journal of the American Chemical Society·Xiao LuoKaifeng Wu

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Citations

Oct 6, 2019·Nature Communications·Lifeng WangKaifeng Wu
Sep 27, 2020·Nanomaterials·Carolina Villamil FrancoElsa Cassette
Nov 17, 2020·Frontiers in Chemistry·James C SadighianCathy Y Wong
Jun 18, 2021·ACS Nano·Amrita DeyLakshminarayana Polavarapu
Jul 13, 2021·Nanoscale·Ivan Marri, Stefano Ossicini
Sep 17, 2019·Journal of the American Chemical Society·In-Hyeok ParkKian Ping Loh
Feb 23, 2020·The Journal of Physical Chemistry Letters·Muyu CongKeli Han
Dec 24, 2019·The Journal of Physical Chemistry Letters·Brener R C ValeJacques-E Moser
Apr 21, 2020·The Journal of Physical Chemistry Letters·Yulu LiKaifeng Wu
Jun 2, 2020·Journal of the American Chemical Society·Xiao LuoKaifeng Wu

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