Attosecond imaging of molecular dynamics
type: Dataset
description: Since the first observation of high-order harmonic spectra in gases, high harmonic generation (HHG) has demonstrated its importance, opening a door to the field of attosecond sience. The bandwidth of the emitted spectrum reaches up to the XUV. The attosecond pulses reach a very high time resolution, allowing the study of electron dynamics in atoms or molecules. The generation mechanism of HHG is based on the emission of an attosecond electron wavepacket by the atoms/molecules. The electron wavepacket is accelerated by the laser field and finally recombines radiatively with its parent ion. Thus the structural information of the probed orbital is encoded in the high harmonic spectrum with a spatial resolution of one Angtröm and a temporal resolution of few femtoseconds. HHG can be used as a probe signal resolved for pump-probe spectroscopy. High harmonic spectroscopy allows the study of the orbital structure and ultra-fast molecular dynamics. In this thesis the fundamental mechanisms playing a role in atoms, molecules and condensed matter are probed using HHG. In order to understand how to extract dynamical and structural information of orbitals from a harmonic signal, we have first studied an easy and well known system: the argon atom. A new theoretical approach developped by Fabre and Pons allowed us to reproduce the experimental results in good agreement. We continued with a study of the molecular structure and dynamics of N2 and CO2. A supersonic Even-Lavie jet permitted to reach rotational temperatures lower than 10K with an excellent alignment distribution. Owing to the good alignment in such gas jet, we were able to resolve the orbital structure with a higher sensitivity and to identify the contribution of several orbitals. In the next step we used the sensitivity of HHG towards the structure of molecular orbitals in order to probe the complex dynamics of NO2 in the vicinity of a conical intersection. We applied HHG combined with transient grating spectroscopy …
landing page: https://theses.hal.science/tel-00803390
keyword: alignement-moleculaire
keyword: atomic
keyword: conical-intersection-attosecond-pulses
keyword: dynamique-moleculaire
keyword: fs-xuv-spectroscopy
keyword: generation-dharmoniques-dordre-eleve
keyword: high-harmonic-spectroscopy
keyword: high-order-harmonic-generation
keyword: impulsions-attosecondes
keyword: infoeu-reposemanticsdoctoralthesis
keyword: interaction-laser-matiere
keyword: intersection-conique
keyword: jet-supersonique
keyword: laser-matter-interaction
keyword: moleculaire-et-des-agregats
keyword: molecular-alignment
keyword: molecular-and-cluster-physics
keyword: molecular-dynamics
keyword: physique-atomique
keyword: physphysphys-atm-phphysics-physicsphysics-physicsatomic-and-molecular-clusters-physicsat
keyword: spectrocopie-harmonique
keyword: spectroscopie-xuv-fs
keyword: supersonic-jet
keyword: theses
issued: 2026-05-12T05:29:52.192477
modified: 2026-05-12T05:29:52.192482
language: en
contact point: Organization
  fn: CCSD

test_moissonnage_selune
type: Agent

Attosecond imaging of molecular dynamics
type: Distribution
format: HTML
access URL: https://theses.hal.science/tel-00803390
issued: 2026-05-12T05:29:52.199398
modified: 2026-05-12T05:29:52.137691