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

Date

Jun 21, 2017

Time

4:30 PM - 5:30 PM

Speaker

Stefanie Gräfe

Affiliation

Universität Jena

Language

en

Main Topic

Physik

Other Topics

Physik

Description

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. In this talk, I will show that the asymmetry in time-resolved photoelectron spectra serves as a tool to distinguish between these dynamics. The influence of an additional, moderately intense infrared (IR) laser field on such asymmetries will be discussed – a pulse combination as it is often applied in attosecond time-resolved experiments. This is done using a simple model for coupled electronic-nuclear motion. The time-resolved photoelectron spectra and their asymmetries directly map the bound electron–nuclear dynamics. From the asymmetries, it is possible to 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. M. Falge, V. Engel, and S. Gräfe, J. Chem. Phys., 2011, 134, 184307 M. Falge, V. Engel, and S. Gräfe., J. Phys. Chem. Lett., 2012, 3, 2617 M. Falge, F. G. Fröbel, V. Engel and S. Gräfe, Phys. Chem. Chem. Phys. 2017, in press.

Last modified: Jun 21, 2017, 9:40:20 AM