Ab initio calculation of femtosecond-time-resolved photoelectron spectra of NO2 after excitation to the A-band.
Andres TehlarAaron von ContaYasuki ArasakiKazuo TakatsukaHans Jakob WörnerPublished in: The Journal of chemical physics (2018)
We present calculations of time-dependent photoelectron spectra of NO2 after excitation to the A-band for comparison with extreme-ultraviolet (XUV) time-resolved photoelectron spectroscopy. We employ newly calculated potential energy surfaces of the two lowest-lying coupled 2A' states obtained from multi-reference configuration-interaction calculations to propagate the photo-excited wave packet using a split-step-operator method. The propagation includes the nonadiabatic coupling of the potential surfaces as well as the explicit interaction with the pump pulse centered at 3.1 eV (400 nm). A semiclassical approach to calculate the time-dependent photoelectron spectrum arising from the ionization to the eight energetically lowest-lying states of the cation allows us to reproduce the static experimental spectrum up to a binding energy of 16 eV and enables direct comparisons with XUV time-resolved photoelectron spectroscopy.
Keyphrases
- density functional theory
- molecular dynamics
- energy transfer
- molecular dynamics simulations
- high resolution
- single molecule
- blood pressure
- monte carlo
- climate change
- biofilm formation
- human health
- risk assessment
- ionic liquid
- electron transfer
- cystic fibrosis
- dna binding
- transcription factor
- gas chromatography
- quantum dots
- clinical evaluation