Simulating pump-probe photo-electron and absorption spectroscopy on the attosecond time-scale with time-dependent density-functional theory
Chemphyschem 14, 1363 - 1376 (2013)
Simulating pump-probe photo-electron and absorption spectroscopy on the attosecond time-scale with time-dependent density-functional theory
Molecular absorption and photo-electron spectra can be efficiently predicted with real-time time-dependent density-functional theory (TDDFT). We show here how these techniques can be easily extended to study time- resolved pump-probe experiments in which a system response (absorption or electron emission) to a probe pulse, is measured in an excited state. This simulation tool helps to interpret the fast evolving attosecond time-resolved spectroscopic experiments, where the electronic motion must be followed at its natural time- scale. We show how the extra degrees of freedom (pump pulse duration, intensity, frequency, and time-delay), which are absent in a conventional steady state experiment, provide additional information about electronic structure and dynamics that improve a system characterization. As an extension of this approach, time- dependent 2D spectroscopies can also be simulated, in principle, for large-scale structures and extended systems.
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- http://dx.doi.org/10.1002/cphc.201201007
- arxiv
- http://arxiv.org/abs/arXiv:1301.1958