Simulating strong-field electron-hole dynamics in solids probed by attosecond transient absorption spectroscopy
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arXiv
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| Format: | Preprint |
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2024
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| author | Cavaletto, Stefano M. Madsen, Lars Bojer |
| author_facet | Cavaletto, Stefano M. Madsen, Lars Bojer |
| contents | We investigate the ultrafast electron dynamics of a model of a wide-bandgap 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 employed 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 TDDFT and SBE-based results allows us to interpret the ab-initio TDDFT simulations in terms of SBEs' interband couplings, validating our SBE-based model and corroborating its conclusions. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2409_01033 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Simulating strong-field electron-hole dynamics in solids probed by attosecond transient absorption spectroscopy Cavaletto, Stefano M. Madsen, Lars Bojer Optics Materials Science Atomic Physics We investigate the ultrafast electron dynamics of a model of a wide-bandgap 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 employed 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 TDDFT and SBE-based results allows us to interpret the ab-initio TDDFT simulations in terms of SBEs' interband couplings, validating our SBE-based model and corroborating its conclusions. |
| title | Simulating strong-field electron-hole dynamics in solids probed by attosecond transient absorption spectroscopy |
| topic | Optics Materials Science Atomic Physics |
| url | https://arxiv.org/abs/2409.01033 |