Time-dependent Hole States in Multiconfigurational Time-Dependent Hartree-Fock Approaches: A Time-Domain Generalization of Extended Koopmans' Theorem
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arXiv
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| Format: | Preprint |
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2025
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| author | Zhang, Zhao-Han Li, Yang Pathak, Himadri Sato, Takeshi Ishikawa, Kenichi L. He, Feng |
| author_facet | Zhang, Zhao-Han Li, Yang Pathak, Himadri Sato, Takeshi Ishikawa, Kenichi L. He, Feng |
| contents | We introduce a framework for resolving electron-hole dynamics within wavefunction-based multiconfigurational time-dependent Hartree-Fock (MCTDHF) theory. Central to this framework is a time-domain generalization of the extended Koopmans' theorem, which rigorously defines time-dependent hole states through single-electron removal. From this foundation, we prove the existence of exact equations of motion for time-dependent Dyson orbitals, enabling instantaneous construction of photofragments' reduced density matrices. The formalism further yields a systematic procedure to extract hole-resolved observables, such as channel-resolved photoelectron momentum distributions, directly from time-dependent \textit{ab initio} wavefunctions. As a demonstration, we employ an attosecond $ω-2ω$ laser strategy to control hole dynamics, thereby resolving a long-standing challenge in MCTDHF simulations. This advance opens a pathway for exploring correlated multielectron dynamics in atoms and molecules under ultrafast laser fields. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2505_11290 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Time-dependent Hole States in Multiconfigurational Time-Dependent Hartree-Fock Approaches: A Time-Domain Generalization of Extended Koopmans' Theorem Zhang, Zhao-Han Li, Yang Pathak, Himadri Sato, Takeshi Ishikawa, Kenichi L. He, Feng Atomic Physics Chemical Physics Quantum Physics We introduce a framework for resolving electron-hole dynamics within wavefunction-based multiconfigurational time-dependent Hartree-Fock (MCTDHF) theory. Central to this framework is a time-domain generalization of the extended Koopmans' theorem, which rigorously defines time-dependent hole states through single-electron removal. From this foundation, we prove the existence of exact equations of motion for time-dependent Dyson orbitals, enabling instantaneous construction of photofragments' reduced density matrices. The formalism further yields a systematic procedure to extract hole-resolved observables, such as channel-resolved photoelectron momentum distributions, directly from time-dependent \textit{ab initio} wavefunctions. As a demonstration, we employ an attosecond $ω-2ω$ laser strategy to control hole dynamics, thereby resolving a long-standing challenge in MCTDHF simulations. This advance opens a pathway for exploring correlated multielectron dynamics in atoms and molecules under ultrafast laser fields. |
| title | Time-dependent Hole States in Multiconfigurational Time-Dependent Hartree-Fock Approaches: A Time-Domain Generalization of Extended Koopmans' Theorem |
| topic | Atomic Physics Chemical Physics Quantum Physics |
| url | https://arxiv.org/abs/2505.11290 |