Simulation and visualization of attosecond stimulated x-ray Raman spectroscopy signals in trans-N-methylacetamide at the nitrogen and oxygen K-edges

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. (C) 2011 American Institute of Physics. [doi:10.1063/1.3557057]