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AbstractQuantum coherence plays a fundamental role in the study and control of ultrafast dynamics in matter. In the case of photoionization, entanglement of the photoelectron with the ion is a well-known source of decoherence when only one of the particles is measured. Here, we investigate decoherence due to entanglement of the radial and angular degrees of freedom of the photoelectron. We study two-photon ionization via the 2s2p autoionizing state in He using high spectral resolution photoelectron interferometry. Combining experiment and theory, we show that the strong dipole coupling of the 2s2p and 2p$$^2$$ states results in the entanglement of the angular and radial degrees of freedom. This translates, in angle-integrated measurements, into a dynamic loss of coherence during autoionization. Graphic Abstract
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High resolution metrology of autoionizing states through Raman interferences
Abstract Metrology of electron wavepackets is often conducted with the technique of photoelectron interferometry. However, the ultrashort light pulses employed in this method place a limit on the energy resolution. Here, weadvance ultrafast photoelectron interferometry access both high temporal and spectral resolution. The key to our approach lies in stimulating Raman interferences with a probe pulse and while monitoring the modification of the autoionizing electron yield in a separate delayed detection step. As a proof of the principle, we demonstrated this technique to obtain the components of an autoionizing nf′ wavepacket between the spin-orbit split ionization thresholds in argon. We extracted the amplitudes and phases from the interferogram and compared the experimental results with second-order perturbation theory calculations. This high resolution probing and metrology of electron dynamics opens the path for study of molecular wavepackets.
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- PAR ID:
- 10429614
- Date Published:
- Journal Name:
- Journal of Physics: Conference Series
- Volume:
- 2494
- Issue:
- 1
- ISSN:
- 1742-6588
- Page Range / eLocation ID:
- 012003
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1088/1742-6596/2494/1/012003
