Attosecond electronic and nuclear quantum photodynamics of ozone monitored with time and angle resolved photoelectron spectra - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue Scientific Reports Année : 2016

Attosecond electronic and nuclear quantum photodynamics of ozone monitored with time and angle resolved photoelectron spectra

Résumé

Recently we reported a series of numerical simulations proving that it is possible in principle to create an electronic wave packet and subsequent electronic motion in a neutral molecule photoexcited by a UV pump pulse within a few femtoseconds. We considered the ozone molecule: for this system the electronic wave packet leads to a dissociation process. In the present work, we investigate more specifically the time-resolved photoelectron angular distribution of the ozone molecule that provides a much more detailed description of the evolution of the electronic wave packet. We thus show that this experimental technique should be able to give access to observing in real time the creation of an electronic wave packet in a neutral molecule and its impact on a chemical process. Since the advent of femtochemistry remarkable and decisive progress has been achieved on the experimental front and it is now possible to monitor electronic motion in the context of attophysics 1-4. In other words, electronic wave packets can be created and observed in real time, which will improve our understanding of fundamental quantum concepts such as coherence and coherent light-matter interaction on the time scale of the electrons in a molecule. Exciting molecules with attosecond XUV light pulses may populate several electronic states coherently, thus creating an electronic molecular wave packet. Its evolution will eventually trigger nuclear motion on a longer timescale via the effective potential created by the electrons and governing nuclear dynamics. In this context, a crucial challenge for attosecond sciences is to create specific electronic wave packets able to induce nuclear motion, e.g. a chemical process, selectively and efficiently. This should lead, on the long term, to what some already call attochemistry, where, at each step of a molecular process, the coupled motions of electrons and nuclei could be controlled on their natural time scales 5. For example, if the attosecond pulse ionizes the molecule , the hole thus created will move, a process which is termed charge migration 5. This may yield, in a second step, to selective bond dissociation 5,6. Another possibility is to populate a limited number of electronic states in the neutral molecule by means of UV subfemtosecond pulses in order to trigger a selective chemical process. Experimentally, attosecond pulses are already available in the XUV spectral domain 7 but few-cycle UV subfem-tosecond pulses are expected to emerge in a near future. A complete theoretical description of such processes is not a trivial task: it requires a quantum mechanical description of both the motion of the electrons and the nuclei in interaction with the external ultrafast field. In previous studies, we presented a full quantum mechanical simulation of the excitation of the ozone (neutral) molecule after excitation by a 3 fs UV pump pulse 8-11. The central wavelength of the pulse at 260 nm was selected so as to create a coherent superposition of only two electronic states: the ground state, X (1 A 1), and the excited B (1 B 2) state 9. The ozone molecule was chosen since, for obvious environmental reasons, its electronic excited states are well-known and understood 12-15. In addition the B state is rather well isolated and, more importantly,
Fichier principal
Vignette du fichier
srep36613.pdf (2.21 Mo) Télécharger le fichier
Origine : Fichiers éditeurs autorisés sur une archive ouverte
Loading...

Dates et versions

hal-01508607 , version 1 (01-07-2020)

Identifiants

Citer

Piero Decleva, Nicola Quadri, Aurelie Perveaux, David Lauvergnat, Fabien Gatti, et al.. Attosecond electronic and nuclear quantum photodynamics of ozone monitored with time and angle resolved photoelectron spectra. Scientific Reports, 2016, 6 (1), ⟨10.1038/srep36613⟩. ⟨hal-01508607⟩
106 Consultations
22 Téléchargements

Altmetric

Partager

Gmail Facebook X LinkedIn More