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dc.contributor.authorMoitra, Torsha
dc.contributor.authorKonecny, Lukas
dc.contributor.authorKadek, Marius
dc.contributor.authorRubio Secades, Angel
dc.contributor.authorRepisky, Michal
dc.identifier.citationThe Journal of Physical Chemistry Letters 14(7) : 1714-1724 (2023)es_ES
dc.description.abstractFirst principles theoretical modeling of out-of-equilibrium processes observed in attosecond pump–probe transient absorption spectroscopy (TAS) triggering pure electron dynamics remains a challenging task, especially for heavy elements and/or core excitations containing fingerprints of scalar and spin–orbit relativistic effects. To address this, we formulate a methodology for simulating TAS within the relativistic real-time, time-dependent density functional theory (RT-TDDFT) framework, for both the valence and core energy regimes. Especially for TAS, full four-component (4c) RT simulations are feasible but computationally demanding. Therefore, in addition to the 4c approach, we also introduce the atomic mean-field exact two-component (amfX2C) Hamiltonian accounting for one- and two-electron picture-change corrections within RT-TDDFT. amfX2C preserves the accuracy of the parent 4c method at a fraction of its computational cost. Finally, we apply the methodology to study valence and near-L2,3-edge TAS processes of experimentally relevant systems and provide additional physical insights using relativistic nonequilibrium response theory.es_ES
dc.description.sponsorshipWe acknowledge the support received from the Research Council of Norway through a Centre of Excellence Grant (no. 262695), a research grant (no. 315822), and mobility grants (nos. 301864 and 314814) as well as the use of computational resources provided by UNINETT Sigma2 – The National Infrastructure for High Performance Computing and Data Storage in Norway (grant no. NN4654K). In addition, this project received funding from the European Union’s Horizon 2020 research and innovation program under Marie Skłodowska-Curie grant agreement no. 945478 (SASPRO2) and the Slovak Research and Development Agency (grant no. APVV-21-0497).es_ES
dc.publisherAmerican Chemical Societyes_ES
dc.titleAccurate Relativistic Real-Time Time-Dependent Density Functional Theory for Valence and Core Attosecond Transient Absorption Spectroscopyes_ES
dc.rights.holder© 2023 The Authors. Published by American Chemical Society. Attribution 4.0 International (CC BY 4.0)es_ES
dc.rights.holderAtribución 3.0 España*
dc.contributor.funderEuropean Commission
dc.departamentoesPolímeros y Materiales Avanzados: Física, Química y Tecnologíaes_ES
dc.departamentoeuPolimero eta Material Aurreratuak: Fisika, Kimika eta Teknologiaes_ES

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© 2023 The Authors. Published by American Chemical Society. Attribution 4.0 International (CC BY 4.0)
Except where otherwise noted, this item's license is described as © 2023 The Authors. Published by American Chemical Society. Attribution 4.0 International (CC BY 4.0)