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X-ray Doppler spectroscopy of ultrafast fragmentation
KTH, Superseded Departments, Biotechnology.
KTH, Superseded Departments, Biotechnology.ORCID iD: 0000-0003-1269-8760
KTH, Superseded Departments, Biotechnology.ORCID iD: 0000-0002-1763-9383
2004 (English)In: Chemical Physics, ISSN 0301-0104, E-ISSN 1873-4421, Chem. Phys., Vol. 299, 253-258 p.Article in journal (Refereed) Published
Abstract [en]

Doppler effects are now commonly observed for Auger resonances of dissociating atoms in randomly oriented molecules. The physics behind the, yet not observed, Doppler effect for fixed-in-space molecules is different in that there will appear extra Doppler resonances resulting from the diffractional scattering of the Auger electrons by the surrounding atoms. It is argued that as these resonances will show maxima in the bond directions their measurement by current energy and angular resolved electron-ion coincidence experiments will provide structural probing. It is also shown that the electronic Doppler effect caused by nuclear vibrations can be observed also for bound nuclear states making use of electron-ion coincidence measurements. Optimal conditions for such measurements prevail when the scattering duration is comparable with a vibrational period.

Place, publisher, year, edition, pages
2004. Vol. 299, 253-258 p.
Keyword [en]
33.70.Ca; 33.80.Eh; 34.50.Gb; Doppler effect; Ultrafast fragmentation; X-ray spectroscopy
National Category
Theoretical Chemistry
URN: urn:nbn:se:kth:diva-5493DOI: 10.1016/j.chemphys.2003.11.017ISI: 000220525200012ScopusID: 2-s2.0-1642414131OAI: diva2:9876
QC 20100906Available from: 2006-03-15 Created: 2006-03-15 Last updated: 2010-09-06Bibliographically approved
In thesis
1. Pulse Propagation in Nonlinear Media and Photonic Crystals
Open this publication in new window or tab >>Pulse Propagation in Nonlinear Media and Photonic Crystals
2006 (English)Doctoral thesis, comprehensive summary (Other scientific)
Abstract [en]

The present thesis is devoted to theoretical studies of pulse propagation of light through linear and nonlinear media, and of light-induced nuclear dynamics.

The first part of the thesis addresses propagation of light pulses in linear periodical media - photonic crystals. The main accent was put on studies of the angular properties of two qualitatively different types of photonic crystals: holographic photonic crystals, and impurity band based photonic crystals. The anisotropy of band structure, group velocity and pulse delay with respect to the light polarization are analyzed.

In the second part of the thesis a strict theory of nonlinear propagation of a few strong interacting light beams is presented. The key idea of this approach is a self-consistent solution of the nonlinear wave equation and the density matrix equations of the material. This technique is applied to studies of dynamics of cavityless lasing generated by ultra-fast multi-photon excitation. It is shown that interaction of co- and counter-propagating pulses of amplified spontaneous emission (ASE) affects the dynamics and efficiency of nonlinear conversion. Our dynamical theory allows to explain the asymmetric spectral properties of the forward and backward ASE pulses, which were observed in recent experiment with different dye molecules. It is shown that the ASE spectral profile changes drastically when the pump intensity approaches the threshold level. The effect of the temporal self-pulsation of ASE is studied in detail.

The third part of the thesis is devoted to light-induced nuclear dynamics. Time- and frequency-resolved X-ray spectroscopy of molecules driven by strong and coherent infrared (IR) pulses shows that the phase of the IR field strongly influences the trajectory of the nuclear wave packet, and hence, the X-ray spectrum. Such a dependence arises due to the interference of one (X-ray) and two-photon (X-ray + IR) excitation channels. The phase of the light influences the dynamics also when the Rabi frequency approaches the vibrational frequency, breaking down the rotating-wave approximation. The probe X-ray spectra are also sensitive to the delay time, the duration, and the shape of the pulses. The evolution of the nuclear wave packets in the dissociative core-excited state affects the dynamics of resonant Auger scattering from fixed-in-space molecules. One of the important dynamical effects is the atomic-like resonance which experiences electronic Doppler shift. We predict that the scattering of the Auger electrons by nearby atoms leads to new Doppler shifted resonances. These extra resonances show sharp maxima in the bond directions, which makes them very promising as probes for local molecular structure using energy and angular resolved electron-ion coincidence techniques. Our theory provides prediction of several new effects, but also results that are in good agreement with the available experimental data.

Place, publisher, year, edition, pages
Stockholm: KTH, 2006. x, 49 p.
Photonic Crystals, Nonlinear optics, X-ray spectroscopy
National Category
Theoretical Chemistry
urn:nbn:se:kth:diva-3886 (URN)91-7178-275-3 (ISBN)
Public defence
2006-03-31, FB42, AlbaNova, Roslagstullsbaken 21, Stockholm, 10:00
QC 20100906Available from: 2006-03-15 Created: 2006-03-15 Last updated: 2011-11-23Bibliographically approved

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