Journal
NANO LETTERS
Volume 20, Issue 3, Pages 1819-1829Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.9b05051
Keywords
Charge-carrier cooling; hot carriers; lead-halide perovskite nanocrystal; electron-phonon coupling excited-states dynamics; nonadiabatic molecular dynamics
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Funding
- Netherlands Organization of Scientific Research (NWO) [723.013.002, 722.017.011]
- BOF UGent
- Marsden Fund
- SURF Cooperative
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We combine state-of-the-art ultrafast photoluminescence and absorption spectroscopy and nonadiabatic molecular dynamics simulations to investigate charge-carrier cooling in CsPbBr3 nanocrystals over a very broad size regime, from 0.8 to 12 nm. Contrary to the prevailing notion that polaron formation slows down charge-carrier cooling in lead-halide perovskites, no suppression of carrier cooling is observed in CsPbBr3 nanocrystals except for a slow cooling (over similar to 10 ps) of warm electrons in the vicinity (within similar to 0.1 eV) of the conduction band edge. At higher excess energies, electrons and holes cool with similar rates, on the order of 1 eV ps(-1) carrier(-1), increasing weakly with size. Our ab initio simulations suggest that cooling proceeds via fast phonon-mediated intraband transitions driven by strong and size-dependent electron-phonon coupling. The presented experimental and computational methods yield the spectrum of involved phonons and may guide the development of devices utilizing hot charge carriers.
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