Jump to main content
Jump to site search
Access to RSC content Close the message box

Continue to access RSC content when you are not at your institution. Follow our step-by-step guide.


Issue 30, 2017
Previous Article Next Article

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

Article information


Submitted
22 Mar 2017
Accepted
26 Apr 2017
First published
28 Apr 2017

Phys. Chem. Chem. Phys., 2017,19, 19683-19690
Article type
Paper

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, 19, 19683
DOI: 10.1039/C7CP01832K

Social activity

Search articles by author

Spotlight

Advertisements