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Photoelectron-recoil-induced rotational excitation of the B 2 state in N2+
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2009 (English)In: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 79, no 022506Article in journal (Refereed) Published
Abstract [en]

In the photoelectron spectrum of N-2 the apparent ionization energy to form the B (2)Sigma(+)(u) state increases linearly with the photon energy. Rotationally resolved measurements of the fluorescent decay of this state show a linear increase of rotational heating with increasing photon energy. These results are in quantitative agreement with the prediction of the theory of recoil-induced rotational excitation, indicating that the rotational heating that has been observed previously arises primarily from such recoil-induced excitation. Together with other results that have been reported they show that recoil-induced internal excitation is significant in many situations, including near threshold.

Place, publisher, year, edition, pages
2009. Vol. 79, no 022506
National Category
Industrial Biotechnology
URN: urn:nbn:se:kth:diva-11436DOI: 10.1103/PhysRevA.79.022506ISI: 000263815000071ScopusID: 2-s2.0-61649092877OAI: diva2:276062

QC 20100713

Available from: 2009-11-10 Created: 2009-11-10 Last updated: 2016-04-22Bibliographically approved
In thesis
1. Molecular electronic,  vibrational and rotational motion in optical and x-ray fields
Open this publication in new window or tab >>Molecular electronic,  vibrational and rotational motion in optical and x-ray fields
2009 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The subject of this theoretical  study is the role ofelectronic structure as well as of rotational and vibrational motionson interactions between molecules and electromagnetic radiation,ranging from optical to x-ray. The thesis concerns both linear and nonlinear regimes of the light-matter interaction. The first part of the thesis is devoted to propagation of opticalpulses with different time-structure through various nonlinear absorbers.First we explain the double-exponential decay of fluorescence caused by photobleaching of pyrylium  salt irradiated by a train of short (100 fs) optical pulses. The main reason for this effect is the transversal inhomogeneity of the light beam which makes the dynamics of the photobleaching differ in the core of the pulse and on its periphery. We also explore the optical power limitingof C60 fullerene irradiated by either microsecond optical pulses or a picosecond pulse trains. Enhancement of nonlinear absorption is caused by strong triplet-triplet absorption that becomes important due toelongation of the interaction time.Here we show the importance of the repetitionrate for the optical power limiting performance.The second part of the thesis addresses the interaction of optical and x-rayfields with rotational degrees of freedom of molecules. In this part the main attention is paid to the rotational heating caused by the recoil, experienced by molecules due to the ejection of photoelectrons. We have quantitatively explained two qualitatively different experiments with the N2 molecule.We predict the interference modulation of the recoil-induced shift,which is a shift of the photoelectron line caused by the rotational recoil effect, as a function of the photon energy.The developed theory also explains the rotational heating ofmolecules observed in the optical fluorescence induced by x-ray radiation.Based on this explanation, we suggest a new scheme of the optical fluorescence induced by x-rays that allows to detect the recoil effect via the recoil-inducedsplitting of the optical resonance.The last part of the thesis focuses on multi-mode nuclear dynamics of the resonant Auger scattering from the C2H2 molecule, that was the subject of a recent experimental study.Here we develop a theory that explains the observed vibrationalscattering anisotropy. We have found that three qualitatively different mechanisms are responsible for this phenomenon. The first mechanism is the interference of the direct and resonance scattering channels. The second mechanismis the interference of the resonant scattering channels through core excitedstate with the orthogonal orientation of the vibrational modes of core excitedstate. The Young's double slit like interference of the quantum pathways through the double-well potential of the bending motion of core excited state is the third mechanism of the vibrational scattering anisotropy.

Place, publisher, year, edition, pages
Stockholm: KTH, 2009. viii, 67 p.
Trita-BIO-Report, ISSN 1654-2312 ; 2009:24
x-ray, nonlinear optics, photobleaching, recoil, anisotropy, Auger
National Category
Atom and Molecular Physics and Optics
urn:nbn:se:kth:diva-11386 (URN)978-91-7415-483-2 (ISBN)
Public defence
2009-12-01, FB 53, AlbaNova, Roslagstullsbacken 21, Stockholm, 10:00 (English)
QC 20100713Available from: 2009-11-10 Created: 2009-11-03 Last updated: 2011-11-23Bibliographically approved

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