Ab initio strong-pump strong-probe doorway-window simulation protocol
Year: 2026
Type: other
Abstract: We have developed an on-the-fly methodology for the simulation ofstrong-field pump-probe (PP) spectra using semiclassical trajectoriesmethods. This methodology generalizes the weak-field semiclassicaldoorway-window (DW) simulation protocol to pump and probe pulses ofany intensity. The strong-field DW functions are defined by explicitanalytical formulas which are fully determined by the molecular transitiondipole moments and electronic energies evaluated along the semiclassicaltrajectories, so that the weak-field and strong-field PP signals canbe simulated at roughly the same computational cost. The developed methodology has been applied for the simulation of strong-field PP spectra ofpyrazine. The obtained results vividly demonstrate the advantage of using strongpump and (notably) probe pulses for increasing the information content of PP measurements. In particular, the strong probe pulse significantlyenhances the weak transitions originating from the lowest excited electronicstates of pyrazine, thereby rendering the nonadiabatic wavepacketdynamics in these weakly allowed states visible.
Source: AIP Publishing
Language: English
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: green
OpenAlex ID: W7168564982