Attosecond interferometry of shape resonances in the recoil frame of CF4
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2021-12-03
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Journal Article
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Abstract
Shape resonances play a central role in many areas of science, but the real-time measurement of the associated many-body dynamics remains challenging. Here, we present measurements of recoil frame angle-resolved photoionization delays in the vicinity of shape resonances of CF4. This technique provides insights into the spatiotemporal photoionization dynamics of molecular shape resonances. We find delays of up to ∼600 as in the ionization out of the highest occupied molecular orbital (HOMO) with a strong dependence on the emission direction and a pronounced asymmetry along the dissociation axis. Comparison with quantum-scattering calculations traces the asymmetries to the interference of a small subset of partial waves at low kinetic energies and, additionally, to the interference of two overlapping shape resonances in the HOMO-1 channel. Our experimental and theoretical results establish a broadly applicable approach to space- and time-resolved photoionization dynamics in the molecular frame.
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7 (49)
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AAAS
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03888 - Wörner, Hans Jakob / Wörner, Hans Jakob
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170775 - Attosecond coincidence spectroscopy of liquids and gases (SNF)
172946 - Soft-X-ray spectroscopy on the attosecond time scale (SNF)
772797 - Attosecond X-ray spectroscopy of liquids (EC)
172946 - Soft-X-ray spectroscopy on the attosecond time scale (SNF)
772797 - Attosecond X-ray spectroscopy of liquids (EC)