基于密度矩阵的含时组态相互作用方法研究超快自旋翻转动力学
Density matrix based time-dependent configuration interaction approach to ultrafast spin-flip dynamics
摘要：
阿秒光谱学的最新发展使人们能够获得电子在其固有时间尺度上的相关运动。自旋翻转动力学通常在价电子态的背景下考虑，其中自旋-轨道耦合较弱，并且与电子自旋相关的过程通常由核运动驱动。然而，对于核心-激发态，其中核心空穴具有非零角动量，自旋轨道耦合足够强以在短得多的时间尺度上驱动自旋翻转。利用基于密度矩阵的含时受限活性空间组态相互作用（包括自旋-轨道耦合），以Fe（II）配合物的L边（2 p $\rightarrow$ 3d）激发态为例，研究了一个前所未有的短自旋交叉.这个过程发生在一个时间尺度上，它比这里明确处理的俄歇衰变（$\sim$ 4\，fs）快。载波频率和脉冲持续时间的适度变化可以导致自旋态产率的实质性变化，这表明其由软X射线光控制。
英文摘要：
Recent developments in attosecond spectroscopy yield access to the correlated motion of electrons on their intrinsic time scales. Spin-flip dynamics is usually considered in the context of valence electronic states, where spin-orbit coupling is weak and processes related to the electron spin are usually driven by nuclear motion. However, for core-excited states, where the core hole has a nonzero angular momentum, spin-orbit coupling is strong enough to drive spin-flips on a much shorter time scale. Using density matrix based time-dependent restricted active space configuration interaction including spin-orbit coupling, we address an unprecedentedly short spin-crossover for the example of L-edge (2p$\rightarrow$3d) excited states of a prototypical Fe(II) complex. This process occurs on a time scale, which is faster than that of Auger decay ($\sim$4\,fs) treated here explicitly. Modest variations of carrier frequency and pulse duration can lead to substantial changes in the spin-state yield, suggesting its control by soft X-ray light.
机构、总结、中文摘要均由AI分析而来，可能存在错误，请以论文正文为准。
