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

Falge M, Froebel FG, Engel V, Gräfe S (2017)

Publication Type: Journal article

Publication year: 2017

Journal

Physical Chemistry Chemical Physics Royal Society of Chemistry

Book Volume: 19

Pages Range: 19683-19690

Journal Issue: 30

DOI: 10.1039/c7cp01832k

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.

Involved external institutions

Julius-Maximilians-Universität Würzburg DE Germany (DE) Friedrich-Schiller-Universität Jena DE Germany (DE)

How to cite

APA:

Falge, M., Froebel, F.G., Engel, V., & Gräfe, S. (2017). Time-resolved photoelectron spectroscopy of IR-driven electron dynamics in a charge transfer model system. Physical Chemistry Chemical Physics, 19(30), 19683-19690. https://doi.org/10.1039/c7cp01832k

MLA:

Falge, Mirjam, et al. "Time-resolved photoelectron spectroscopy of IR-driven electron dynamics in a charge transfer model system." Physical Chemistry Chemical Physics 19.30 (2017): 19683-19690.

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