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Quantum wave packet revivals in IR plus X-ray pump-probe spectroscopy
KTH, School of Biotechnology (BIO), Theoretical Chemistry (closed 20110512).
KTH, School of Biotechnology (BIO), Theoretical Chemistry (closed 20110512).
KTH, School of Biotechnology (BIO), Theoretical Chemistry (closed 20110512).ORCID iD: 0000-0002-1763-9383
2005 (English)In: Chemical Physics Letters, ISSN 0009-2614, E-ISSN 1873-4448, Vol. 405, no 4-6, 398-403 p.Article in journal (Refereed) Published
Abstract [en]

The wave packet revivals constitute a central concept of X-ray spectroscopy with ultra-high spectral resolution. The revival phenomenon allows to resolve the anharmonical shift or rotational structure by means of time dependent measurements and makes X-ray pump-probe spectroscopy a powerful technique to study long-term dynamics of molecules in different phases. We study the revivals referring to the X-ray absorption spectrum of the NO molecule driven by strong infrared pulse. It is shown that the phase sensitive trajectories of the center of gravity of the wave packets and the X-ray spectra copy each other.

Place, publisher, year, edition, pages
Elsevier, 2005. Vol. 405, no 4-6, 398-403 p.
Keyword [en]
Absorption, Infrared spectroscopy, Molecular structure, X ray analysis
National Category
Theoretical Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-5651DOI: 10.1016/j.cplett.2005.02.061ISI: 000228207100029Scopus ID: 2-s2.0-15944369971OAI: oai:DiVA.org:kth-5651DiVA: diva2:10089
Note

QC 20100825

Available from: 2006-05-05 Created: 2006-05-05 Last updated: 2016-07-22Bibliographically 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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Ågren, Hans

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