2021/12/22 by Umberto De Giovannini, Shunsuke A. Sato, Shunsuke Sato +3
Engineering · Physics and Astronomy · #Advanced Chemical Physics Studies #Angle-resolved photoemission spectroscopy #Computational physics #Computer science #Density functional theory #Electronic structure #Excitation #Molecular Junctions and Nanostructures #Observable #Physics #Quantum mechanics #Scalability #Spectroscopy and Quantum Chemical Studies #cond-mat.mtrl-sci
paper · pdf · doi:10.1016/j.elspec.2021.147152
openalex publication_date 2021/12/22 · arxiv created 2021/12/24 · arxiv updated 2021/12/28 · openalex created_date 2025/10/10 · openalex updated_date 2026/08/06
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.