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Pump-probe spectroscopy of molecules driven by infrared field in both ground and excited electronic states
KTH, School of Biotechnology (BIO), Theoretical Chemistry (closed 20110512).
KTH, School of Biotechnology (BIO), Theoretical Chemistry (closed 20110512).
2006 (English)In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 125, no 20, 204313Article in journal (Refereed) Published
Abstract [en]

Pump-probe spectra of molecules driven by strong infrared (IR) field in both ground and excited states are studied theoretically. The role of the final state interaction becomes important when pump and probe pulses overlap, and the Rabi frequency is comparable with the lifetime broadening of the excited state and the duration of the pump pulse. Our theoretical approach is applied to x-ray absorption of nitrogen molecule and valence photoionization of carbon monoxide. It is shown that IR-x-ray pump-probe spectroscopy can directly evidence the delocalization of core hole.

Place, publisher, year, edition, pages
American Institute of Physics (AIP), 2006. Vol. 125, no 20, 204313
Keyword [en]
vibrational wave-functions; packet revivals; ray; radiation; spectra; o2
National Category
Theoretical Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-5655DOI: 10.1063/1.2393234ISI: 000242408100027PubMedID: 17144706Scopus ID: 2-s2.0-33751569874OAI: oai:DiVA.org:kth-5655DiVA: diva2:10093
Note

Uppdaterad från manuskript till artikel: 20100825 Tidigare titel: Pump-probe spectroscopy of molecules driven by IR field in both ground and excited states QC 20100825

Available from: 2006-05-05 Created: 2006-05-05 Last updated: 2017-12-14Bibliographically approved
In thesis
1. X-ray Spectroscopy of Molecules Driven by Strong IR Fields
Open this publication in new window or tab >>X-ray Spectroscopy of Molecules Driven by Strong IR Fields
2006 (English)Doctoral thesis, comprehensive summary (Other scientific)
Abstract [en]

The current thesis deals with one important branch of the physics of ultrafast processes, namely modeling of femtosecond nuclear dynamics. We suggest a new type of time resolved spectroscopy, the phase sensitive infrared-x-ray pump probe spectroscopy, which combines rich opportunities of IR laser techniques in quantum control of molecular systems with the site selectivity of x-rays. We have developed and applied a dynamical theory of x-ray pump-probe spectroscopy to study different molecular systems. Special attention is paid to design of the wave packets of desirable shape and spectral composition. Such a quantum control of the nuclear wave packet enables the study of molecular properties in regions that are unavailable by standard x-ray spectroscopies. The IR - x-ray pump probe spectroscopy is nicely suited to perform mapping of wave packet trajectories, to study revival phenomena, femtosecond chemical dynamics, and proton transfer, to mention a few examples.

Our simulations show that the phase of the infrared pulse strongly influences the trajectory of the nuclear wave packet, and hence, the x-ray spectrum. Such a dependence is caused by the transfer of the phase of the IR field to the wave packet through the interference of the one (x-ray) and two-photon (IR + x-ray) excitation channels. The time resolved x-ray spectra are sensitive to the shape, duration and delay time between the pulses. The phase of the IR pulse influences the molecular dynamics also when the Rabi period becomes comparable with the period of vibrations, breaking down the rotating wave approximation. We predict a phase memory effect which is a promising technique in studies of chemical dynamics on different time scales. It is shown that the final state interaction with the pump affects the probe spectrum when the pump and probe pulses overlap.

In a further step, we explore the electronic recoil effect in x-ray photoelectron spectroscopy, which has recently attracted attention of experimentalists due to its sensitivity to intramolecular interaction. We show that an IR field enhances the manifestation of the recoil effect through the formation of extensive vibrational wave packets. The theory of x-ray Raman scattering from molecules with strong spin-orbit coupling accompanied by electron-hole interaction is developed and applied to simulations of resonant x-ray Raman scattering of the HCl molecule. Special attention is paid to the theoretical methodologies to reduce the computational cost of our wave packet codes.

Place, publisher, year, edition, pages
Stockholm: KTH, 2006. ix, 53 p.
National Category
Theoretical Chemistry
Identifiers
urn:nbn:se:kth:diva-3937 (URN)91-7178-277-X (ISBN)
Public defence
2006-05-19, Sal FR4, AlbaNova Universitetscentrum, Roglagstullsbacken 21, Stochholm, 10:00
Opponent
Supervisors
Note
QC 20100825Available from: 2006-05-05 Created: 2006-05-05 Last updated: 2011-11-23Bibliographically approved

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