Jump to main content
Jump to site search


Time-resolved photoelectron spectroscopy of IR-driven electron dynamics in a charge transfer model system

Author affiliations

Abstract

If the adiabatic approximation is valid, electrons smoothly adapt to molecular geometry changes. In contrast, as a characteristic of diabatic dynamics, the electron density does not follow the nuclear motion. Recently, we have shown that the asymmetry in time-resolved photoelectron spectra serves as a tool to distinguish between these dynamics [Falge et al., J. Phys. Chem. Lett., 2012, 3, 2617]. Here, we investigate the influence of an additional, moderately intense infrared (IR) laser field, as often applied in attosecond time-resolved experiments, on such asymmetries. This is done using a simple model for coupled electronic-nuclear motion. We calculate time-resolved photoelectron spectra and their asymmetries and demonstrate that the spectra directly map the bound electron–nuclear dynamics. From the asymmetries, we can trace the IR field-induced population transfer and both the field-driven and intrinsic (non-)adiabatic dynamics. This holds true when considering superposition states accompanied by electronic coherences. The latter are observable in the asymmetries for sufficiently short XUV pulses to coherently probe the coupled states. It is thus documented that the asymmetry is a measure for phases in bound electron wave packets and non-adiabatic dynamics.

Graphical abstract: Time-resolved photoelectron spectroscopy of IR-driven electron dynamics in a charge transfer model system

Back to tab navigation

Publication details

The article was received on 22 Mar 2017, accepted on 26 Apr 2017 and first published on 28 Apr 2017


Article type: Paper
DOI: 10.1039/C7CP01832K
Citation: Phys. Chem. Chem. Phys., 2017, Advance Article
  •   Request permissions

    Time-resolved photoelectron spectroscopy of IR-driven electron dynamics in a charge transfer model system

    M. Falge, F. G. Fröbel, V. Engel and S. Gräfe, Phys. Chem. Chem. Phys., 2017, Advance Article , DOI: 10.1039/C7CP01832K

Search articles by author

Spotlight

Advertisements