Attosecond interferometry of shape resonances in the recoil frame of CF(4).
Attosecond interferometry of shape resonances in the recoil frame of CF(4).
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DOI:
10.1126/sciadv.abj8121
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发表时间:
2021-12-03
期刊:
影响因子:
13.6
通讯作者:
Wörner HJ
中科院分区:
文献类型:
--
作者:
Heck S;Baykusheva D;Han M;Ji JB;Perry C;Gong X;Wörner HJ
This study reports fully angle- and state-resolved measurement of time delays in molecular photoionization. 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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