Abstract
Motivated by the possibility of multiphoton-driven pump-probe experiments, such as time-resolved photoelectron spectroscopy, we carry out essential states's calculations of strong-field molecular excitation by solving the time-dependent Schrödinger equation for a molecule in a high-intensity laser field. Usually such calculations rely on adiabatic elimination, but here we make direct use of a large number of energies and transition dipole moments obtained from electronic structure calculations. In this way, we capture a range of multiphoton absorption orders, from 2 to 5, and include dynamic Stark shifts naturally. We consider a range of laser frequencies and intensities to characterize several multiphoton resonances and dynamic Stark shifts. The calculations also include averaging over molecular orientation and geometry, but are carried out for frozen nuclei, which is relevant in the limit of very short laser pulses (
Original language | English |
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Article number | 013111 |
Number of pages | 10 |
Journal | Physical Review A |
Volume | 106 |
Issue number | 1 |
DOIs | |
Publication status | Published - 19 Jul 2022 |
Austrian Fields of Science 2012
- 103036 Theoretical physics
- 104022 Theoretical chemistry
- 102009 Computer simulation
Keywords
- ANO BASIS-SETS
- INTERNAL-CONVERSION
- THIOPHENE
- SPECTROSCOPY
- DYNAMICS
- PROGRAM
- OLIGOTHIOPHENES
- STATES