Ultrafast dynamics of hot carriers: Theoretical approaches based on real-time propagation of carrier distributions
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Date
2025-02-14
Authors
Sjakste, Jelena
Sen, Raja
Vast, Nathalie
Saint-Martin, Jerome
Ghanem, Mohammad
Dollfus, Philippe
Murphy-Armando, Felipe
Kanasaki, Junichi
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American Institute of Physics
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Abstract
In recent years, computational approaches which couple density functional theory (DFT)-based description of the electron–phonon and phonon–phonon scattering rates with the Boltzmann transport equation have been shown to obtain the electron and thermal transport characteristics of many 3D and 2D semiconductors in excellent agreement with experimental measurements. At the same time, progress in the DFT-based description of the electron–phonon scattering has also allowed to describe the non-equilibrium relaxation dynamics of hot or photo-excited electrons in several materials, in very good agreement with time-resolved spectroscopy experiments. In the latter case, as the time-resolved spectroscopy techniques provide the possibility to monitor transient material characteristics evolving on the femtosecond and attosecond time scales, the time evolution of photo-excited, nonthermal carrier distributions has to be described. Similarly, reliable theoretical approaches are needed to describe the transient transport properties of devices involving high energy carriers. In this review, we aim to discuss recent progress in coupling the ab initio description of materials, especially that of the electron–phonon scattering, with the time-dependent approaches describing the time evolution of the out-of-equilibrium carrier distributions, in the context of time-resolved spectroscopy experiments as well as in the context of transport simulations. We point out the computational limitations common to all numerical approaches, which describe time propagation of strongly out-of-equilibrium carrier distributions in 3D materials, and discuss the methods used to overcome them.
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Keywords
Density functional theory (DFT) , 3D materials , Hot carrier , Carrier distribution
Citation
Sjakste, J., Sen, R., Vast, N., Saint-Martin, J., Ghanem, M., Dollfus, P., Murphy-Armando, F. and Kanasaki, J. (2025) 'Ultrafast dynamics of hot carriers: Theoretical approaches based on real-time propagation of carrier distributions', Journal of Chemical Physics, 162(6), 061002. https://doi.org/10.1063/5.0245834
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© 2025, the Authors. Published under an exclusive license by AIP Publishing. This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing.