2024-03-28T19:42:28Zhttp://digital.csic.es/dspace-oai/requestoai:digital.csic.es:10261/950642019-02-21T09:09:25Zcom_10261_115com_10261_3col_10261_368
Giovannini, Umberto de
Brunetto, Gustavo
Castro, Alberto
Walkenhorst, Jessica
Rubio, Angel
2014-04-07T09:32:03Z
2014-04-07T09:32:03Z
2013
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
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.
eng
openAccess
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
artículo