论文标题
多原子分子的核心价值瞬时吸收光谱
Core-valence attosecond transient absorption spectroscopy of polyatomic molecules
论文作者
论文摘要
追踪通过光与物质相互作用引起的超快过程通常非常具有挑战性。在分子系统中，最初创建的电子相干性通过飞秒时间尺度上缓慢的核重排而抑制，这使得分子中电子动力学的实时观察特别困难。在这项工作中，我们报告了分子案例的AttoSecond瞬时吸收光谱（ATA）的理论的扩展，其中包括对最初创建的波数据包中耦合的电子 - 核动力学的完整说明，并将其应用于外在含量抗价酸离子酸分子的阳性电荷的振荡。通过利用X射线辐射引起的元素特异性核心到价转变，我们表明ATA的分辨率使得可以通过原子空间分辨率跟踪电子密度的动力学。
Tracing ultrafast processes induced by interaction of light with matter is often very challenging. In molecular systems, the initially created electronic coherence becomes damped by the slow nuclear rearrangement on a femtosecond timescale which makes real-time observations of electron dynamics in molecules particularly difficult. In this work, we report an extension of the theory underlying the attosecond transient absorption spectroscopy (ATAS) for the case of molecules, including a full account for the coupled electron-nuclear dynamics in the initially created wave packet, and apply it to probe the oscillations of the positive charge created after outer-valence ionization of the propiolic acid molecule. By taking advantage of element-specific core-to-valence transitions induced by X-ray radiation, we show that the resolution of ATAS makes it possible to trace the dynamics of electron density with atomic spatial resolution.
