6533b82cfe1ef96bd12900ab
RESEARCH PRODUCT
First-principles modelling for time-resolved ARPES under different pump-probe conditions
Umberto De GiovanniniShunsuke A. SatoHannes HübenerAngel Rubiosubject
Time-resolved angular resolved photoelectron spectroscopy (ARPES)Condensed Matter - Materials ScienceRadiationMaterials Science (cond-mat.mtrl-sci)FOS: Physical sciences02 engineering and technologyTheoretical spectroscopy021001 nanoscience & nanotechnologyCondensed Matter Physics01 natural sciencesAtomic and Molecular Physics and OpticsSettore FIS/03 - Fisica Della MateriaElectronic Optical and Magnetic MaterialsComputational methods for excitation in solids0103 physical sciencesTime-dependent density functional theoryPhysical and Theoretical Chemistry010306 general physics0210 nano-technologySpectroscopydescription
First-principles methods for time-resolved angular resolved photoelectron spectroscopy play a pivotal role in providing interpretation and microscopic understanding of the complex experimental data and in exploring novel observables or observation conditions that may be achieved in future experiments. Here we describe an efficient, reliable and scalable first-principles method for tr-ARPES based on time-dependent density functional theory including propagation and surface effects usually discarded in the widely used many-body techniques based on computing the non-equilibrium spectral function and discuss its application to a variety of pump–probe conditions. We identify four conditions, depending on the length of the probe relative to the excitation in the materials on the one hand and on the overlap between pump and probe on the other hand. Within this paradigm different examples of observables of time-resolved ARPES are discussed in view of the newly developed and highly accurate time-resolved experimental spectroscopies.
| year | journal | country | edition | language |
|---|---|---|---|---|
| 2021-12-24 |