Time-dependent Hole States in Multiconfigurational Time-Dependent Hartree-Fock Approaches: Applications in Photoionization of Water Molecule
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| Main Authors: | , , , , , |
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| Format: | Preprint |
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2025
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| _version_ | 1866909988109156352 |
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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 | By simulating the real-time multielectron wavefunction with the multi-configurational time-dependent Hartree-Fock (MCTDHF) approach, we conduct an \textit{ab initio} study of the single-photon ionization process of a body-fixed water molecule ($\mathrm{H_2O}$) driven by attosecond pulses. To this end, we present a full-dimensional implementation of the MCTDHF method based on one-center expansions, allowing for the simulation of arbitrarily polarized lasers and multi-center polyatomic potentials. With a rigorous definition of the time-dependent hole state (TDHS) using the time-domain generalization of extended Koopmans' theorem (TD-EKT), we derive the reduced ion density matrix within the MCTDHF framework, which inherently encodes the total and channel-resolved photoionization cross sections of $\mathrm{H_2O}$. The cross sections obtained are benchmarked against existing experimental and theoretical results, validating the TDHS formalism. Furthermore, by adjusting the phase delay and intensity ratio of a pair of orthogonally polarized attosecond pulses, we explore the ultrafast control of attosecond coherence between electronic states of $\mathrm{H_2O^+}$. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2505_11319 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Time-dependent Hole States in Multiconfigurational Time-Dependent Hartree-Fock Approaches: Applications in Photoionization of Water Molecule Zhang, Zhao-Han Li, Yang Pathak, Himadri Sato, Takeshi Ishikawa, Kenichi L. He, Feng Atomic Physics Chemical Physics Quantum Physics By simulating the real-time multielectron wavefunction with the multi-configurational time-dependent Hartree-Fock (MCTDHF) approach, we conduct an \textit{ab initio} study of the single-photon ionization process of a body-fixed water molecule ($\mathrm{H_2O}$) driven by attosecond pulses. To this end, we present a full-dimensional implementation of the MCTDHF method based on one-center expansions, allowing for the simulation of arbitrarily polarized lasers and multi-center polyatomic potentials. With a rigorous definition of the time-dependent hole state (TDHS) using the time-domain generalization of extended Koopmans' theorem (TD-EKT), we derive the reduced ion density matrix within the MCTDHF framework, which inherently encodes the total and channel-resolved photoionization cross sections of $\mathrm{H_2O}$. The cross sections obtained are benchmarked against existing experimental and theoretical results, validating the TDHS formalism. Furthermore, by adjusting the phase delay and intensity ratio of a pair of orthogonally polarized attosecond pulses, we explore the ultrafast control of attosecond coherence between electronic states of $\mathrm{H_2O^+}$. |
| title | Time-dependent Hole States in Multiconfigurational Time-Dependent Hartree-Fock Approaches: Applications in Photoionization of Water Molecule |
| topic | Atomic Physics Chemical Physics Quantum Physics |
| url | https://arxiv.org/abs/2505.11319 |