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  Laser-induced modification of an excited-state vibrational wave packet in neutral H2 observed in a pump-control scheme

Borisova, G. D., Barber Belda, P., Hu, S., Birk, P., Stooss, V., Hartmann, M., et al. (2024). Laser-induced modification of an excited-state vibrational wave packet in neutral H2 observed in a pump-control scheme. Physical Review Research, 6(3): 033326. doi:10.1103/PhysRevResearch.6.033326.

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Borisova, Gergana D.1, Author                 
Barber Belda, Paula1, Author                 
Hu, Shuyuan1, Author           
Birk, Paul1, Author                 
Stooss, Veit1, Author           
Hartmann, Maximilian1, Author                 
Fan, Daniel1, Author           
Moshammer, Robert1, Author                 
Saenz, Alejandro, Author
Ott, Christian1, Author                 
Pfeifer, Thomas1, Author                 
Affiliations:
1Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society, ou_2025284              

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Free keywords: Dipole approximation,High-harmonic generation, Molecular dynamics, Schroedinger equation, Transient absorption spectroscopy, Molecules, Atomic & molecular processes in external fields, Coherent control, Electronic transitions, Few-cycle light pulses, Ultrashort pulses, Vibrational states, Vibronic effects
 Abstract: We observe and modify a molecular vibrational wave packet in an electronically excited state of the neutral hydrogen molecule. In an extreme-ultraviolet (XUV) time-domain absorption spectroscopy experiment, we launch a vibrational wave packet in the D1Πu3pn state of H2 and track its time evolution via the coherent dipole response. The reconstructed time-dependent dipole from experimentally measured XUV absorption spectra provides access to the revival of the vibrational wave packet, which we control via an intense near-infrared (NIR) pulse. Tuning the intensity of the NIR pulse, we observe the revival of the wave packet to be significantly modified, which is supported by the results of a multilevel simulation as well as an analytical model based on state-specific phase shifts. The NIR field is applied only 7 fs after the creation of the wave packet but influences its evolution up to at least its first revival at 270 fs. This experimental approach for nonlocal-in-time laser modification of quantum dynamics in a pump-control scheme enabled by molecular self-probing is generally applicable to a large range of molecules and materials as it only requires the observation of absorption spectra.

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 Dates: 2024-09-23
 Publication Status: Published online
 Pages: 10
 Publishing info: -
 Table of Contents: -
 Rev. Type: -
 Identifiers: DOI: 10.1103/PhysRevResearch.6.033326
 Degree: -

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Title: Physical Review Research
  Abbreviation : Phys. Rev. Research
Source Genre: Journal
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Publ. Info: College Park, Maryland, United States : American Physical Society (APS)
Pages: - Volume / Issue: 6 (3) Sequence Number: 033326 Start / End Page: - Identifier: ISSN: 2643-1564
CoNE: https://pure.mpg.de/cone/journals/resource/2643-1564