Electronic relaxation dynamics of a metal atom deposited on argon cluster
type: Distribution
access URL: https://theses.hal.science/tel-00985781
format: HTML
issued: 2026-05-05T12:31:26.847900
modified: 2026-05-05T12:31:26.815513

Electronic relaxation dynamics of a metal atom deposited on argon cluster
type: Dataset
contact point: Organization
  fn: CCSD
keyword: molecular-dynamics
keyword: pseudopotential
keyword: dynamique-moleculaire
keyword: quantum-chemistry
keyword: optimisation-des-structures
keyword: femtochemistry
keyword: femtochimie
keyword: ab-initio-method
keyword: chimie-quantique
keyword: dynamique-reactionnelle
keyword: physcondcm-genphysics-physicscondensed-matter-cond-matother-cond-matother
keyword: metaux
keyword: pseudopotentiel
keyword: theses
keyword: spectroscopie-dabsorption
keyword: methode-ab-initio
keyword: chimothechemical-sciencesother
keyword: infoeu-reposemanticsdoctoralthesis
keyword: optimization-of-the-structures
keyword: absorption-spectroscopy
keyword: metals
keyword: reactional-dynamics
landing page: https://theses.hal.science/tel-00985781
description: This thesis is a study on the interaction between electronically excited atomic states and a non-reactive environment. We have theoretically and experimentally studied situations where a metal atom (Ba or K) is placed in a finite size environment (argon cluster). The presence of the medium affects the electronic levels of the atom. On the other side, the excitation of the atom induces a relaxation dynamics of the electronic energy through the deformation of the cluster. The experimental part of this work focuses on two aspects : the spectroscopy and the dynamics. In both cases a first laser electronically excites the metal atom and the second ionizes the excited system. The observable is the photoelectron spectrum recorded after photoionization and possibly information on the photoion which are also produced. This pump/probe technique, with also two lasers, provide the ultrafast dynamic when the lasers pulses used are of ultrashort (60 fs ). The use of nanosecond lasers leads to resonance spectroscopic measurement, unresolved temporally, which give information on the position of the energy levels of the studied system. From a theoretical point-of-view, the excited states of M-Ar_n were calculated at the ab initio level, using large core pseudo-potential to limit the active electrons of the metal to valence electrons. The study of alkali metals (potassium) is especially well adapted to this method since only one electron is active. The ab-initio calculation and a Monte-Carlo simulation where coupled to optimize the geometry of the KAr_n (n = 1-10) cluster when K is in the ground state of the neutral and the ion, or excited in the 4p or 5s state. Calculations were also conducted in collaboration with B. Gervais (CIMAP, Caen) on KAr_n clusters having several tens of argon atoms. Absorption spectra were also calculated. From an experimental point-of-view, we were able to characterize the excited states of potassium and barium perturbed by the clusters. In both cases a b…
identifier: NNT: 2014PA112013
issued: 2026-05-05T12:31:26.844599
language: fr
modified: 2026-05-05T12:31:26.844604

test_moissonnage_selune
type: Agent