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Enhancement of the recoil effect in x-ray photoelectron spectra of molecules driven by a strong ir field
KTH, Skolan för bioteknologi (BIO), Teoretisk kemi (stängd 20110512).
KTH, Skolan för bioteknologi (BIO), Teoretisk kemi (stängd 20110512).
KTH, Skolan för bioteknologi (BIO), Teoretisk kemi (stängd 20110512).
2005 (Engelska)Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 72, nr 2, s. 023414-Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

The C K and O K x-ray photoelectron spectra of the CO molecule, driven by a strong ir field, are studied theoretically. An enhancement of the recoil effect, which results in a strong dependence of the electron vibrational profile on the energy of x-ray photon, is found. The enhancement of the recoil effect happens due to an ir-induced increase of the wave-packet size. An extra enhancement occurs when the gradients of ground and ionized states approach each other. Under an increase of the photon energy, different sides of the x-ray photoelectron band experience blue- and redshifts, which are related to the difference of the gradients of the ground and core ionized states in the points of the vertical transitions near turning points of the wave packet. This makes the ir-x-ray pump-probe spectroscopy a very promising tool to study the shape of the potential energy surfaces.

Ort, förlag, år, upplaga, sidor
2005. Vol. 72, nr 2, s. 023414-
Nyckelord [en]
basis-sets, spectroscopy, propagation, probe, esca, co
Nationell ämneskategori
Kemi
Identifikatorer
URN: urn:nbn:se:kth:diva-5652DOI: 10.1103/PhysRevA.72.023414ISI: 000231564200143Scopus ID: 2-s2.0-27144472945OAI: oai:DiVA.org:kth-5652DiVA, id: diva2:10090
Anmärkning

QC 20100825

Tillgänglig från: 2006-05-05 Skapad: 2006-05-05 Senast uppdaterad: 2017-12-14Bibliografiskt granskad
Ingår i avhandling
1. X-ray Spectroscopy of Molecules Driven by Strong IR Fields
Öppna denna publikation i ny flik eller fönster >>X-ray Spectroscopy of Molecules Driven by Strong IR Fields
2006 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
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.

Ort, förlag, år, upplaga, sidor
Stockholm: KTH, 2006. s. ix, 53
Nationell ämneskategori
Teoretisk kemi
Identifikatorer
urn:nbn:se:kth:diva-3937 (URN)91-7178-277-X (ISBN)
Disputation
2006-05-19, Sal FR4, AlbaNova Universitetscentrum, Roglagstullsbacken 21, Stochholm, 10:00
Opponent
Handledare
Anmärkning
QC 20100825Tillgänglig från: 2006-05-05 Skapad: 2006-05-05 Senast uppdaterad: 2011-11-23Bibliografiskt granskad

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Felicissimo, Viviane C.Guimaraes, Freddy FernandesGelmukhanov, Faris
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Teoretisk kemi (stängd 20110512)
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Physical Review A. Atomic, Molecular, and Optical Physics
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