Thermalization and relaxation mediated by phonon management in tin-lead perovskites

Linjie Dai; Junzhi Ye; Neil C. Greenham

doi:10.1038/s41377-023-01236-w

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Thermalization and relaxation mediated by phonon management in tin-lead perovskites

Original Articles

- Thermalization and relaxation mediated by phonon management in tin-lead perovskites
- Light: Science & Applications Vol. 12, Issue 9, Pages: 1971-1981(2023)
- Affiliations：
  
  Cavendish Laboratory, University of Cambridge, 19 J. J. Thomson Avenue, Cambridge CB3 0HE, UK
- Author bio：
  
  Neil C. Greenham (ncg11@cam.ac.uk)
- Funds：
- DOI：10.1038/s41377-023-01236-w
  CLC：
- Published：30 September 2023，
  
  Published Online：30 August 2023，
  
  Received：18 January 2023，
  
  Revised：04 July 2023，
  
  Accepted：14 July 2023
- Accepted：
Scan QR Code
Dai, L. J., Ye, J. Z. & Greenham, N. C. Thermalization and relaxation mediated by phonon management in tin-lead perovskites. Light: Science & Applications, 12, 1971-1981 (2023).
DOI：

Dai, L. J., Ye, J. Z. & Greenham, N. C. Thermalization and relaxation mediated by phonon management in tin-lead perovskites. Light: Science & Applications, 12, 1971-1981 (2023). DOI： 10.1038/s41377-023-01236-w.

摘要

Abstract

Understanding and control of ultrafast non-equilibrium processes in semiconductors is key to making use of the full photon energy before relaxation

leading to new ways to break efficiency limits for solar energy conversion. In this work

we demonstrate the observation and modulation of slow relaxation in uniformly mixed ti

n-lead perovskites (MASn

1-x

and CsSn

1-x

nanocrystals). Transient absorption measurements reveal that slow cooling mediated by a hot phonon bottleneck effect appears at carrier densities above ~10

−3

for tin-lead alloy nanocrystals

and tin addition is found to give rise to suppressed cooling. Within the alloy nanoparticles

the combination of a newly introduced high-energy band

screened Fröhlich interaction

suppressed Klemens decay and reduced thermal conductivity (acoustic phonon transport) with increased tin content contributes to the slowed relaxation. For inorganic nanocrystals where defect states couple strongly with carriers

sodium doping has been confirmed to benefit in maintaining hot carriers by decoupling them from deep defects

leading to a decreased energy-loss rate during thermalization and an enhanced hot phonon bottleneck effect. The slow cooling we observe uncovers the intrinsic photophysics of perovskite nanocrystals

with implications for photovoltaic applications where suppressed cooling could lead to hot-carrier solar cells.

关键词

Keywords

references

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