Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule
Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule
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DOI：
10.1103/physrevx.11.031048
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发表时间：
2021-09-01
影响因子：
12.5
通讯作者：
Kolorenc, P.
中科院分区：
文献类型：
--
作者：
Barillot, T.;Alexander, O.;Kolorenc, P.
突然电离的分子在显著的结构变化之前经历极快的电子空穴（或空穴）动力学的可能性在20多年前首次被认识到，并被称为电荷迁移。超快电子空穴动力学的精确探测需要具有足够的时间分辨率并且可以检测分子内特定空穴的定位的测量。我们报告的调查，在异丙醇中，我们使用的X-射线泵浦-X-射线探测实验，与现场和特定状态的探测定位在分子中的氧原子附近的瞬态空穴态的内部价空穴态的动力学，连同从头算理论处理。我们记录了瞬态孔动力学的签名，并首次尝试性地观察了受挫折的Auger-Meitner转换驱动的动力学。我们验证了有效空穴寿命与我们的理论预测是一致的。这种状态特定的测量铺平了道路，广泛应用于观察瞬态空穴动力学定位在空间和时间的分子，从而电荷转移现象，是化学和材料物理学的基础。
The possibility of suddenly ionized molecules undergoing extremely fast electron hole (or hole) dynamics prior to significant structural change was first recognized more than 20 years ago and termed charge migration. The accurate probing of ultrafast electron hole dynamics requires measurements that have both sufficient temporal resolution and can detect the localization of a specific hole within the molecule. We report an investigation of the dynamics of inner valence hole states in isopropanol where we use an x-ray pump-x-ray probe experiment, with site and state-specific probing of a transient hole state localized near the oxygen atom in the molecule, together with an ab initio theoretical treatment. We record the signature of transient hole dynamics and make the first tentative observation of dynamics driven by frustrated Auger-Meitner transitions. We verify that the effective hole lifetime is consistent with our theoretical prediction. This state-specific measurement paves the way to widespread application for observations of transient hole dynamics localized in space and time in molecules and thus to charge transfer phenomena that are fundamental in chemical and material physics.