2024-03-28T12:12:51Zhttp://digital.csic.es/dspace-oai/requestoai:digital.csic.es:10261/950642019-02-21T09:09:25Zcom_10261_115com_10261_3col_10261_368
00925njm 22002777a 4500
dc
Giovannini, Umberto de
author
Brunetto, Gustavo
author
Castro, Alberto
author
Walkenhorst, Jessica
author
Rubio, Angel
author
2013
Molecular absorption and photoelectron spectra can be efficiently predicted with real-time time-dependent density functional theory. We show herein 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 with the interpretation of fast-evolving attosecond time-resolved spectroscopic experiments, in which electronic motion must be followed at its natural timescale. 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 characterization of a system. As an extension of this approach, time-dependent 2D spectroscopy can also be simulated, in principle, for large-scale structures and extended systems. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
ChemPhysChem 14(7): 1363-1376 (2013)
http://hdl.handle.net/10261/95064
10.1002/cphc.201201007
http://dx.doi.org/10.13039/501100000781
http://dx.doi.org/10.13039/501100000780
http://dx.doi.org/10.13039/501100006366
ab initio calculations
Time-resolved spectroscopy
Attosecond dynamics
Single-molecule studies
Laser spectroscopy
Simulating pump-probe photoelectron and absorption spectroscopy on the attosecond timescale with time-dependent density functional theory