Simulating strong-field electron-hole dynamics in solids probed by attosecond transient absorption spectroscopy

We investigate the ultrafast electron dynamics of a model of a wide-band-gap material with inner, valence, and conduction bands excited by an intense few-femtosecond pump and monitored by a delayed attosecond extreme-ultraviolet probe pulse. Complementary computational methods are utilized and compared, based on the semiconductor Bloch equations (SBEs) and time-dependent density functional theory (TDDFT). TDDFT is employed to study a finite-size system, while the SBEs are utilized to investigate the corresponding solid with periodic boundary conditions imposed, with the crystal-momentum-dependent energy bands and interband couplings calculated in the parallel-transport structure gauge. The resulting strong-field electron dynamics are used to predict experimentally accessible attosecond transient absorption spectroscopy (ATAS) signals as a function of the probe-pulse frequency and pump-probe interpulse delay. Both simulation protocols similarly capture the time-delay-dependent spectral features in the ATAS signals. The very good agreement between our ab initio TDDFT simulations and SBE-based results allows us to validate our SBE-based model and identify the key contributing interband couplings. An interpretation model building on these validated SBE-based results allows us to quantify the amplitude of the ATAS spectral features in terms of the intraband dynamics of the electron-hole pairs generated by the attosecond probe pulse.

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Publication Details

Journal
Physical review. A/Physical review, A
Published
2024-11-25
DOI
https://doi.org/10.1103/physreva.110.053111
Citations
2
Primary Topic
Laser-Matter Interactions and Applications
Type
article
Field-Weighted Citation Impact
0.68

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article

Simulating strong-field electron-hole dynamics in solids probed by attosecond transient absorption spectroscopy

Lars Bojer Madsen, Stefano M. Cavaletto
2 citations
Physical review. A/Physical review, A
Laser-Matter Interactions and Applications
0.68
article

Simulating strong-field electron-hole dynamics in solids probed by attosecond transient absorption spectroscopy

Lars Bojer Madsen, Stefano M. Cavaletto
article en
2 citations

Abstract

We investigate the ultrafast electron dynamics of a model of a wide-band-gap material with inner, valence, and conduction bands excited by an intense few-femtosecond pump and monitored by a delayed attosecond extreme-ultraviolet probe pulse. Complementary computational methods are utilized and compared, based on the semiconductor Bloch equations (SBEs) and time-dependent density functional theory (TDDFT). TDDFT is employed to study a finite-size system, while the SBEs are utilized to investigate the corresponding solid with periodic boundary conditions imposed, with the crystal-momentum-dependent energy bands and interband couplings calculated in the parallel-transport structure gauge. The resulting strong-field electron dynamics are used to predict experimentally accessible attosecond transient absorption spectroscopy (ATAS) signals as a function of the probe-pulse frequency and pump-probe interpulse delay. Both simulation protocols similarly capture the time-delay-dependent spectral features in the ATAS signals. The very good agreement between our ab initio TDDFT simulations and SBE-based results allows us to validate our SBE-based model and identify the key contributing interband couplings. An interpretation model building on these validated SBE-based results allows us to quantify the amplitude of the ATAS spectral features in terms of the intraband dynamics of the electron-hole pairs generated by the attosecond probe pulse.

Physical review. A/Physical review, AVol. 110(5)
Aarhus University (DK)
H2020 Marie Skłodowska-Curie Actions
Affordable and clean energy
Openalex Percentile: Top 30%
Laser-Matter Interactions and Applications
0.68
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