Disentangling conical intersection and coherent molecular dynamics in methyl bromide with attosecond transient absorption spectroscopy
Disentangling conical intersection and coherent molecular dynamics in methyl bromide with attosecond transient absorption spectroscopy
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DOI：
10.1038/s41467-019-10789-7
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发表时间：
2019-07
影响因子：
16.6
通讯作者：
H. Timmers;Xiaolei Zhu;Zheng Li;Yuki Kobayashi;M. Sabbar;M. Hollstein;Maurizio Reduzzi;T. Martínez;D. Neumark;S. Leone
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文献类型：
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作者：
H. Timmers;Xiaolei Zhu;Zheng Li;Yuki Kobayashi;M. Sabbar;M. Hollstein;Maurizio Reduzzi;T. Martínez;D. Neumark;S. Leone
阿秒探测核能级的电子跃迁提供了一个敏感的工具，研究原子，状态和电荷特异性的价分子动力学。在这份报告中，我们采用阿秒瞬态吸收光谱跟踪强场引发的溴甲烷过程的价态动力学。通过对3d核-价跃迁的探测，我们解决了溴甲烷中性σ ~* 激发态的强场激发和随后的碎裂问题。结果提供了一个明确的签名的非绝热通过的激发态波包通过一个圆锥形的交叉。我们还观察到竞争，强场引发的过程中产生的基态和电离分子对应的振动和自旋轨道运动，分别。所展示的解决具有几个飞秒分辨率的同步动力学的能力，为阿秒XUV光谱作为探测具有无与伦比的时间分辨率的竞争和复杂分子现象的通用工具的实施提供了一条明确的前进道路。
Attosecond probing of core-level electronic transitions provides a sensitive tool for studying valence molecular dynamics with atomic, state, and charge specificity. In this report, we employ attosecond transient absorption spectroscopy to follow the valence dynamics of strong-field initiated processes in methyl bromide. By probing the 3dcore-to-valence transition, we resolve the strong field excitation and ensuing fragmentation of the neutralσ* excited states of methyl bromide. The results provide a clear signature of the non-adiabatic passage of the excited state wavepacket through a conical intersection. We additionally observe competing, strong field initiated processes arising in both the ground state and ionized molecule corresponding to vibrational and spin-orbit motion, respectively. The demonstrated ability to resolve simultaneous dynamics with few-femtosecond resolution presents a clear path forward in the implementation of attosecond XUV spectroscopy as a general tool for probing competing and complex molecular phenomena with unmatched temporal resolution.