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Phonon-mediated and weakly size-dependent electron and hole cooling in CsPbBr3 nanocrystals revealed by atomistic simulations and ultrafast spectroscopy

(2020) NANO LETTERS. 20(3). p.1819-1829
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Abstract
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.
Keywords
Mechanical Engineering, General Materials Science, Bioengineering, General Chemistry, Condensed Matter Physics

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MLA
Boehme, Simon C., et al. “Phonon-Mediated and Weakly Size-Dependent Electron and Hole Cooling in CsPbBr3 Nanocrystals Revealed by Atomistic Simulations and Ultrafast Spectroscopy.” NANO LETTERS, vol. 20, no. 3, 2020, pp. 1819–29.
APA
Boehme, S. C., ten Brinck, S., Maes, J., Yazdani, N., Zapata, F., Chen, K., … Infante, I. (2020). Phonon-mediated and weakly size-dependent electron and hole cooling in CsPbBr3 nanocrystals revealed by atomistic simulations and ultrafast spectroscopy. NANO LETTERS, 20(3), 1819–1829.
Chicago author-date
Boehme, Simon C., Stephanie ten Brinck, Jorick Maes, Nuri Yazdani, Felipe Zapata, Kai Chen, Vanessa Wood, et al. 2020. “Phonon-Mediated and Weakly Size-Dependent Electron and Hole Cooling in CsPbBr3 Nanocrystals Revealed by Atomistic Simulations and Ultrafast Spectroscopy.” NANO LETTERS 20 (3): 1819–29.
Chicago author-date (all authors)
Boehme, Simon C., Stephanie ten Brinck, Jorick Maes, Nuri Yazdani, Felipe Zapata, Kai Chen, Vanessa Wood, Justin M. Hodgkiss, Zeger Hens, Pieter Geiregat, and Ivan Infante. 2020. “Phonon-Mediated and Weakly Size-Dependent Electron and Hole Cooling in CsPbBr3 Nanocrystals Revealed by Atomistic Simulations and Ultrafast Spectroscopy.” NANO LETTERS 20 (3): 1819–1829.
Vancouver
1.
Boehme SC, ten Brinck S, Maes J, Yazdani N, Zapata F, Chen K, et al. Phonon-mediated and weakly size-dependent electron and hole cooling in CsPbBr3 nanocrystals revealed by atomistic simulations and ultrafast spectroscopy. NANO LETTERS. 2020;20(3):1819–29.
IEEE
[1]
S. C. Boehme et al., “Phonon-mediated and weakly size-dependent electron and hole cooling in CsPbBr3 nanocrystals revealed by atomistic simulations and ultrafast spectroscopy,” NANO LETTERS, vol. 20, no. 3, pp. 1819–1829, 2020.
@article{8648405,
  abstract     = {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.},
  author       = {Boehme, Simon C. and ten Brinck, Stephanie and Maes, Jorick and Yazdani, Nuri and Zapata, Felipe and Chen, Kai and Wood, Vanessa and Hodgkiss, Justin M. and Hens, Zeger and Geiregat, Pieter and Infante, Ivan},
  issn         = {1530-6984},
  journal      = {NANO LETTERS},
  keywords     = {Mechanical Engineering,General Materials Science,Bioengineering,General Chemistry,Condensed Matter Physics},
  language     = {eng},
  number       = {3},
  pages        = {1819--1829},
  title        = {Phonon-mediated and weakly size-dependent electron and hole cooling in CsPbBr3 nanocrystals revealed by atomistic simulations and ultrafast spectroscopy},
  url          = {http://dx.doi.org/10.1021/acs.nanolett.9b05051},
  volume       = {20},
  year         = {2020},
}

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