Department of Chemistry, University of California, Irvine, California 92697-2025, USA.
J Chem Phys. 2011 Mar 28;134(12):124101. doi: 10.1063/1.3557057.
The stimulated Raman component of the pump-probe spectrum of trans-N-methylacetamide obtained in response to two soft x-ray pulses is calculated by treating the core excitations at the Hartree-Fock static-exchange level. The signal reveals the dynamics of valence-electron wave packets prepared and detected in the vicinity of a selected atom (either nitrogen or oxygen). The evolving electronic charge density as well as electronic coherence of the doorway and the window created by the two pulses are visualized using a time-dependent basis set of natural orbitals, which reveals that the wave packets consist of several entangled valence particle-hole pairs.
采用哈特ree-fock 静态交换水平处理核心激发，计算了反式-n-甲基乙酰胺的泵浦探测光谱中受两个软 x 射线脉冲激发的受激拉曼分量。该信号揭示了在选定原子（氮或氧）附近制备和检测的价电子波包的动力学。通过使用自然轨道的时变基组，直观地显示了由两个脉冲产生的门和窗口的演化电子电荷密度和电子相干性，这表明波包由几个纠缠的价粒子-空穴对组成。
