Investigation of Ultrafast Molecular Dynamics via Covariance Mapping: A Tool for Intense XUV Light Sources

Research output: ThesisDoctoral Thesis (compilation)


The study of molecular dynamics involves observations of the motion of nuclei and electrons. While nuclear motion is usually on the picosecond or femtosecond timescale, attosecond precision is necessary to directly observe the motion of electrons. Ultrashort laser pulses have become established as a viable tool for probing femtosecond dynamics by irradiating the target for only extremely short times. This allows snapshots of the motion to be obtained. However, extreme ultraviolet (XUV) or soft X-ray wavelengths are required to generate attosecond pulses. Two light sources that produce ultrashort XUV pulses were used during the work presented in this thesis: the free electron laser in Hamburg (FLASH) and the high-order harmonic generation-based light source at the High-Intensity XUV Beamline in Lund.

This thesis describes the application of covariance mapping and pump-probe spectroscopy as tools to investigate molecular dynamics at these XUV light sources. A covariance mapping scheme was implemented in conjunction with a double-sided velocity map imaging spectrometer at the High-Intensity XUV Beamline. Its capabilities were demonstrated in a proof-of-principle experiment on molecular nitrogen. The scheme was subsequently applied to more complex molecules, and results from photoion-photoion covariance mapping of adamantane (C10H16) are presented. The photodissociation behavior of halomethane molecules was investigated with infrared - ultraviolet and ultraviolet - soft X-ray pump-probe schemes during several measurement campaigns at FLASH. While these time-resolved experiments probed dynamics mainly on the picosecond timescale, efforts were made at the High-Intensity XUV Beamline towards attosecond precision XUV-XUV pump-probe experiments. After demonstrating the ability to induce two-photon processes with XUV light, the XUV wavefronts were studied over several experimental campaigns. These campaigns led to a significant reduction of aberrations in the XUV wavefronts. The size and quality of the XUV focal spot as well as the XUV generation yield were improved.


  • Jan Lahl
Research areas and keywords

Subject classification (UKÄ) – MANDATORY

  • Atom and Molecular Physics and Optics


  • Covariance, Ultrafast, High-order harmonic generation, Extreme Ultraviolet, Pump probe, FLASH, Velocity map imaging, wavefront, FEL, photodissociation, Coulomb explosion, Fysicumarkivet A:2019:Lahl
Original languageEnglish
Awarding Institution
Supervisors/Assistant supervisor
Award date2019 Mar 29
Place of PublicationLund
  • Department of Physics, Lund University
Print ISBNs978-91-7753-976-6
Electronic ISBNs978-91-7753-977-3
Publication statusPublished - 2019 Mar 4
Publication categoryResearch

Bibliographic note

Defence details Date: 2019-03-29 Time: 13:15 Place: Rydbergsalen, Fysicum, Professorsgatan 1, Lund University, Faculty of Engineering LTH External reviewer(s) Name: Veisz, Lázsló Title: Professor Affiliation: Umeå University, Sweden ---

Total downloads

No data available

Related research output

Dacasa, H., Coudert-alteirac, H., Chen Guo, Kueny, E., Campi, F., Lahl, J., Peschel, J., Wikmark, H., Major, B., Erik Malm, Alj, D., Varjú, K., Cord L. Arnold, Dovillaire, G., Per Johnsson, Anne L’huillier, Maclot, S., Rudawski, P. & Zeitoun, P., 2019 Feb 4, In : Optics Express. 27, 3, p. 2656-2670

Research output: Contribution to journalArticle

Allum, F., Burt, M., Amini, K., Boll, R., Köckert, H., Olshin, P. K., Bari, S., Bomme, C., Brauße, F., Cunha de Miranda, B., Düsterer, S., Erk, B., Géléoc, M., Geneaux, R., Gentleman, A. S., Goldsztejn, G., Guillemin, R., Holland, D. M. P., Ismail, I., Johnsson, P. & 30 others, Journel, L., Küpper, J., Lahl, J., Lee, J. W. L., Maclot, S., Mackenzie, S. R., Manschwetus, B., Mereshchenko, A. S., Mason, R., Palaudoux, J., Piancastelli, M. N., Penent, F., Rompotis, D., Rouzée, A., Ruchon, T., Rudenko, A., Savelyev, E., Simon, M., Schirmel, N., Stapelfeldt, H., Techert, S., Travnikova, O., Trippel, S., Underwood, J. G., Vallance, C., Wiese, J., Ziaee, F., Brouard, M., Marchenko, T. & Rolles, D., 2018 Nov 28, In : Journal of Chemical Physics. 149, 20, p. 204313

Research output: Contribution to journalArticle

Rading, L., Lahl, J., Maclot, S., Campi, F., Coudert-Alteirac, H., Oostenrijk, B., Peschel, J., Wikmark, H., Rudawski, P., Mathieu Gisselbrecht & Per Johnsson, 2018 Jun 19, In : Applied Sciences (Switzerland). 8, 6, 998.

Research output: Contribution to journalArticle

View all (7)