Probing vibronic coherence in charge migration in molecules using strong-field sequential double ionization

Yuen, C. H.; Lin, C. D.

doi:10.1103/physreva.109.l011101

Phys. Rev. A

2024

DOI: 10.1103/physreva.109.l011101

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Probing vibronic coherence in charge migration in molecules using strong-field sequential double ionization

C. H. Yuen,

C. D. Lin

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2024

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Cited by 4 publications

References 36 publications

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Rotation in attosecond vibronic coherence spectroscopy for molecules

Yuen,

Lin

2024

Commun Phys

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Excitation or ionization of a molecule by ultrafast laser pulses can create a superposition of electronic states, whose dynamics is influenced by the interplay of electronic coherence and nuclear motion, resulting in charge migration and possibly charge transfer. Probing the vibronic coherence is therefore vital to monitoring electronic dynamics and controlling chemical reactivity, as recently demonstrated in molecules via attosecond transient absorption spectroscopy (ATAS). However, theories supporting the interpretation of ATAS experiments neglect the effects of molecular rotation, often leading to inaccurate interpretation of experimental data. Here, we develop a comprehensive theory for ATAS of molecules encompassing the entire pump-probe process. Applying the theory to N2, we demonstrate that the emergence of coherent signals critically depends on the consideration of molecular rotation. This work contributes to close the gap between theory and ATAS experiments, paving the way for monitoring electronic motion and controlling chemical reactivity in diverse molecular systems.

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Rotation in attosecond vibronic coherence spectroscopy for molecules

Yuen,

Lin

2024

Commun Phys

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Relativistic treatment of hole alignment in noble gas atoms

Tahouri,

Papoulia,

Carlström

et al. 2024

Commun Phys

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The development in attosecond physics allows for unprecedented control of atoms and molecules in the time domain. Here, ultrashort pulses are used to prepare atomic ions in specific magnetic states, which may be important for controlling charge migration in molecules. Our work fills the knowledge gap of relativistic hole alignment prepared by femtosecond and attosecond pulses. The research focuses on optimizing the central frequency and duration of pulses to exploit specific spectral features, such as Fano profiles, Cooper minima, and giant resonances. Simulations are performed using the Relativistic Time-Dependent Configuration-Interaction Singles method. Ultrafast hole alignment with large ratios (on the order of one hundred) is observed in the outer-shell hole of argon. An even larger alignment (on the order of one thousand) is observed in the inner-shell hole of xenon.

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Theory of strong-field sequential double ionization of polyatomic molecules

Yuen,

Lin

2024

Phys. Rev. A

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Probing vibronic coherence in charge migration in molecules using strong-field sequential double ionization

Cited by 4 publications

References 36 publications

Rotation in attosecond vibronic coherence spectroscopy for molecules

Rotation in attosecond vibronic coherence spectroscopy for molecules

Relativistic treatment of hole alignment in noble gas atoms

Theory of strong-field sequential double ionization of polyatomic molecules

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