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
Wörner HJ
中科院分区:
综合性期刊1区
文献类型:
--
作者:
Heck S;Baykusheva D;Han M;Ji JB;Perry C;Gong X;Wörner HJ

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这项研究报告了分子光电离时间延迟的完全角度和状态分辨测量。形状共振在许多科学领域发挥着核心作用,但相关多体动力学的实时测量仍然具有挑战性。在这里,我们展示了 CF4 形状共振附近反冲框架角分辨光电离延迟的测量结果。该技术提供了对分子形状共振的时空光电离动力学的见解。我们发现最高占据分子轨道 (HOMO) 的电离延迟高达 ∼600,这对发射方向有很强的依赖性,并且沿解离轴具有明显的不对称性。与量子散射计算的比较将不对称性追溯到低动能部分波的小子集的干扰,此外,还追溯到 HOMO-1 通道中两个重叠形状共振的干扰。我们的实验和理论结果建立了一种广泛适用的分子框架中空间和时间分辨光电离动力学的方法。
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.
DOI: 10.1063/1.467237
发表时间: 1994-05-01
影响因子: 4.4
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