6533b859fe1ef96bd12b776e
RESEARCH PRODUCT
Simulating pump-probe photo-electron and absorption spectroscopy on the attosecond time-scale with time-dependent density-functional theory
Andrea CastroJessica WalkenhorstGustavo BrunettoGustavo BrunettoAngel RubioAngel RubioAngel RubioUmberto De Giovanninisubject
Time-resolved spectroscopyTime FactorsAbsorption spectroscopyAtomic Physics (physics.atom-ph)AttosecondAttosecond dynamicsFOS: Physical sciencesPump probesingle-molecule studies01 natural sciencestime-resolved spectroscopySettore FIS/03 - Fisica Della MateriaPhysics - Atomic PhysicsAb initio quantum chemistry methodsPhysics - Chemical Physics0103 physical sciencesPhysics - Atomic and Molecular ClustersLaser spectroscopyPhysical and Theoretical Chemistry010306 general physicsSpectroscopyPhysicsChemical Physics (physics.chem-ph)010304 chemical physicsEuropean researchab initio calculationsPhotoelectron SpectroscopySingle-molecule studiesattosecond dynamicsTime-dependent density functional theoryAtomic and Molecular Physics and OpticsPhysics - Plasma PhysicsPlasma Physics (physics.plasm-ph)X-Ray Absorption Spectroscopylaser spectroscopyQuantum TheoryAtomic physicsTime-resolved spectroscopyAtomic and Molecular Clusters (physics.atm-clus)description
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.
| year | journal | country | edition | language |
|---|---|---|---|---|
| 2013-03-20 |