Journal
CHEMPHYSCHEM
Volume 14, Issue 7, Pages 1363-1376Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.201201007
Keywords
ab initio calculations; attosecond dynamics; laser spectroscopy; single-molecule studies; time-resolved spectroscopy
Funding
- European Research Council Advanced Grant DYNamo [267374]
- ACI-Promociona [ACI2009-1036]
- Grupos Consolidados UPV/EHU del Gobierno Vasco [IT-319-07]
- European Commission [280879-2 CRONOS CP-FP7, 228539]
- CAPES Foundation
- Ministry of Education of Brazil [2287/110]
- [FIS2011-65702-C02-01]
- [PIB2010US-00652]
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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 pumpprobe 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.
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