论文标题
X射线诱导的Tropone的超热非绝热动力学中的种群陷阱在O（1 \ textit {s}）pre-Edge处探测
Population Trap in X-ray-induced Ultrafast Nonadiabatic Dynamics of Tropone Probed at the O(1\textit{s}) pre-edge
论文作者
论文摘要
非绝热过渡（NAT）驱动了自然界和各个领域中使用的各种X射线诱导的光化学和光体物理学。为了阐明X射线诱导的NAT动力学，我们对由碳$ kll $正常促进剂衰减产生的电子激发型型（TR）进行了非绝热分子动力学模拟。 Tr $^{2+} $通过10-10 $^2 $状态经历NAT CASCADE，其时间常数为200-400 fs。我们观察到NAT级联过程中100 FS的高度激发态中的种群陷阱。该人群陷阱的指纹可以从C（$ 1S $）边缘泵O（$ 1S $）的前边缘探针proge pripe flstsecond瞬态X射线吸收光谱中，该X射线吸收光谱通过O（$ 1S $）凸台钻机电子产量方法（TR-EAPAE）使用强烈的狭窄狭窄的Band band famtosecond famtosecond X射线X射线X射线X射线pulses。我们的耦合电离速率方程模型表明，TR的选择性和饱和C（$ 1S $）核心离子化实现了无背景测量。这些结果表明，NAT在大分子中的X射线光化学和光体物理学的重要性。使用TR-EAYS对NAT动力学的实时跟踪对于更深入的洞察力应是一种有力的方法。
Nonadiabatic transition (NAT) drives a variety of x-ray-induced photochemistry and photophysics used in nature and various fields. To clarify the x-ray-induced NAT dynamics, we performed nonadiabatic molecular dynamics simulations on electronically excited tropone (Tr) dications created by the carbon $KLL$ normal Auger decay. The Tr$^{2+}$ undergoes the NAT cascade via 10-10$^2$ states with time constants of 200-400 fs. We observed population traps in the highly excited states in 100 fs during the NAT cascade. The fingerprint of this population trap can be extracted from C($1s$) edge pump O($1s$) pre-edge probe femtosecond transient x-ray absorption spectra measured by the O($1s$) Auger electron yield method (TR-AEYS) using intense narrow band femtosecond x-ray free electron laser pulses. Our coupled ionization rate equation model demonstrates that selective and saturable C($1s$) core-ionization of Tr realizes background-free measurement. These results indicate that the importance of NAT in x-ray photochemistry and photophysics in large molecules. The real-time tracking of the NAT dynamics using TR-AEYS shall be a powerful approach for deeper insight.
