Technical review: Time-dependent density functional theory for attosecond physics ranging from gas-phase to solids

Abstract First-principles electron dynamics calculations can be applied in the investigation of a wide range of ultrafast phenomena in attosecond physics. They offer unique microscopic insight into light-induced ultrafast phenomena in both gas and condensed phases of matter, and thus, they are a pow...

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Main Authors: Shunsuke A. Sato, Hannes Hübener, Umberto De Giovannini, Angel Rubio
Format: Article
Language:English
Published: Nature Portfolio 2025-07-01
Series:npj Computational Materials
Online Access:https://doi.org/10.1038/s41524-025-01715-1
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author Shunsuke A. Sato
Hannes Hübener
Umberto De Giovannini
Angel Rubio
author_facet Shunsuke A. Sato
Hannes Hübener
Umberto De Giovannini
Angel Rubio
author_sort Shunsuke A. Sato
collection DOAJ
description Abstract First-principles electron dynamics calculations can be applied in the investigation of a wide range of ultrafast phenomena in attosecond physics. They offer unique microscopic insight into light-induced ultrafast phenomena in both gas and condensed phases of matter, and thus, they are a powerful tool to develop our understanding of the physics of attosecond phenomena. We specifically review techniques employing time-dependent density functional theory (TDDFT) for investigating attosecond and strong-field phenomena. First, we describe this theoretical framework that enables the modeling of perturbative and non-perturbative electron dynamics in materials, including atoms, molecules, and solids. We then discuss its application to attosecond experiments, focusing on the reconstruction of attosecond beating by interference of two-photon transitions (RABBIT) measurements. We also briefly review first-principles calculations of optical properties of solids with TDDFT in the linear response regime and their extension to calculations of transient optical properties of solids in non-equilibrium phases, by simulating experimental pump-probe setups. We further demonstrate the application of TDDFT simulation to high-order harmonic generation in solids. First-principles calculations have predictive power, and hence they can be utilized to design future experiments to explore non-equilibrium and nonlinear ultrafast phenomena in matter and characterize and control metastable light-induced quantum states.
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spelling doaj-art-3d2ef240dcb4495285e94d1b62d7bc282025-08-20T03:46:23ZengNature Portfolionpj Computational Materials2057-39602025-07-0111111110.1038/s41524-025-01715-1Technical review: Time-dependent density functional theory for attosecond physics ranging from gas-phase to solidsShunsuke A. Sato0Hannes Hübener1Umberto De Giovannini2Angel Rubio3Department of Physics, Tohoku UniversityMax Planck Institute for the Structure and Dynamics of Matter and Center for Free Electron Laser ScienceMax Planck Institute for the Structure and Dynamics of Matter and Center for Free Electron Laser ScienceMax Planck Institute for the Structure and Dynamics of Matter and Center for Free Electron Laser ScienceAbstract First-principles electron dynamics calculations can be applied in the investigation of a wide range of ultrafast phenomena in attosecond physics. They offer unique microscopic insight into light-induced ultrafast phenomena in both gas and condensed phases of matter, and thus, they are a powerful tool to develop our understanding of the physics of attosecond phenomena. We specifically review techniques employing time-dependent density functional theory (TDDFT) for investigating attosecond and strong-field phenomena. First, we describe this theoretical framework that enables the modeling of perturbative and non-perturbative electron dynamics in materials, including atoms, molecules, and solids. We then discuss its application to attosecond experiments, focusing on the reconstruction of attosecond beating by interference of two-photon transitions (RABBIT) measurements. We also briefly review first-principles calculations of optical properties of solids with TDDFT in the linear response regime and their extension to calculations of transient optical properties of solids in non-equilibrium phases, by simulating experimental pump-probe setups. We further demonstrate the application of TDDFT simulation to high-order harmonic generation in solids. First-principles calculations have predictive power, and hence they can be utilized to design future experiments to explore non-equilibrium and nonlinear ultrafast phenomena in matter and characterize and control metastable light-induced quantum states.https://doi.org/10.1038/s41524-025-01715-1
spellingShingle Shunsuke A. Sato
Hannes Hübener
Umberto De Giovannini
Angel Rubio
Technical review: Time-dependent density functional theory for attosecond physics ranging from gas-phase to solids
npj Computational Materials
title Technical review: Time-dependent density functional theory for attosecond physics ranging from gas-phase to solids
title_full Technical review: Time-dependent density functional theory for attosecond physics ranging from gas-phase to solids
title_fullStr Technical review: Time-dependent density functional theory for attosecond physics ranging from gas-phase to solids
title_full_unstemmed Technical review: Time-dependent density functional theory for attosecond physics ranging from gas-phase to solids
title_short Technical review: Time-dependent density functional theory for attosecond physics ranging from gas-phase to solids
title_sort technical review time dependent density functional theory for attosecond physics ranging from gas phase to solids
url https://doi.org/10.1038/s41524-025-01715-1
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