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

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Borisova,  Gergana D.       
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Barber Belda,  Paula       
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Hu,  Shuyuan
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Birk,  Paul       
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Stooss,  Veit
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Hartmann,  Maximilian       
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Fan,  Daniel
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Moshammer,  Robert       
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Ott,  Christian       
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Pfeifer,  Thomas       
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Citation

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.


Cite as: https://hdl.handle.net/21.11116/0000-000F-E983-6
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.