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Attosecond interferometry of shape resonances in the recoil frame of CF4.

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.

SUBMITTER: Heck S 

PROVIDER: S-EPMC8641934 | biostudies-literature | 2021 Dec

REPOSITORIES: biostudies-literature

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Attosecond interferometry of shape resonances in the recoil frame of CF<sub>4</sub>.

Heck Saijoscha S   Baykusheva Denitsa D   Han Meng M   Ji Jia-Bao JB   Perry Conaill C   Gong Xiaochun X   Wörner Hans Jakob HJ  

Science advances 20211203 49

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 CF<sub>4</sub>. 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 (  ...[more]

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