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Wave packet theory of resonant X-ray scattering
KTH, Superseded Departments, Biotechnology.
2001 (English)Doctoral thesis, comprehensive summary (Other scientific)
Place, publisher, year, edition, pages
Stockholm: KTH , 2001. , x, 43 p.
Keyword [en]
RXS, x-ray scattering, wave packets
National Category
Engineering and Technology
Identifiers
URN: urn:nbn:se:kth:diva-3188ISBN: 91-7283-111-1 (print)OAI: oai:DiVA.org:kth-3188DiVA: diva2:8957
Public defence
2001-06-11, 00:00
Note
QC 20100629Available from: 2001-06-08 Created: 2001-06-08 Last updated: 2010-06-30Bibliographically approved
List of papers
1. Duration of x-ray Raman scattering
Open this publication in new window or tab >>Duration of x-ray Raman scattering
1999 (English)In: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 59, no 1, 380-389 p.Article in journal (Refereed) Published
Abstract [en]

There has recently been much interest in using the notion of a duration time to analyze resonant x-ray Raman scattering (RXS) of atoms, molecules, and solids. This notion implies a selection of processes with different time scales responsible for the formation x-ray Raman spectra, and has been useful for actual predictions of various phenomena associated with RXS and that subsequently have been experimentally verified. However, the notion of a duration time for the x-ray scattering event can also have some paradoxical consequences, as when comparing the RXS duration with the relaxation time of the wave packet evolution in the case when the inverse detuning of the excitation energy is shorter than the time of flight or the lifetime of the core excited state. We present here a solution of this contradiction and give a detailed analysis of the notion of the duration time for RXS. It is shown that this time is complex and consists of two qualitatively different contributions. The first originates in the irreversible decay of the core excited state, while the imaginary part is caused by a reversible dephasing in the time domain. We investigate also the evolution of the wave packets of bound and dissociative states to stationary distributions. The theoretical analysis is accompanied by numerical examples of the time evolution of the wave packet in bound and dissociative core excited states of the N2 and HCl molecules.

National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-13608 (URN)10.1103/PhysRevA.59.380 (DOI)
Note
QC 20100622Available from: 2010-06-22 Created: 2010-06-22 Last updated: 2017-12-12Bibliographically approved
2. Wave-packet dynamics of resonant x-ray Raman scattering: Excitation near the Cl L-II,L-III edge of HCl
Open this publication in new window or tab >>Wave-packet dynamics of resonant x-ray Raman scattering: Excitation near the Cl L-II,L-III edge of HCl
1999 (English)In: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 59, no 2, 1147-1159 p.Article in journal (Refereed) Published
Abstract [en]

A theory of radiative and nonradiative x-ray Raman scattering based on nuclear wave-packet dynamics is presented. The theory is evaluated with special emphasis on the cases when the intermediate and/or final state potentials are dissociative. Different "one-step" and "two-step" time-dependent wave-packet formalisms are proposed and evaluated, giving different interpretational content and computational efficiency. An interference between the molecular background and the narrow atomiclike contributions is predicted and evaluated. Due to this interference the atomiclike spectral feature manifests itself as a peak or as a spectral hole depending on the circumstances in terms of excitation energy, spectral width of incident radiation, and the form of the interatomic potentials. The counterintuitive situation may even arise that a narrow peak is formed by increasing the spectral photon width. The duration of the resonant x-ray Raman scattering influences in a qualitatively different manner the space distributions of the wave packets in the molecular and the dissociative domains, something that is crucial for the formation of the cross section profile. It is shown that the scattering cross section is proportional to the square of the core excited wave packet and inversely proportional to the derivative of the difference between core excited and final state potentials. The atomiclike profile is shown to consist of a Lorentzian inner part and red or blue wings which give direct information about the long-range regions of the potentials; red wings for diverging potentials, and blue for converging. A technique of mapping of the space distribution of the squared core excited wave packet and the interatomic potentials is suggested. The various features are demonstrated by an ab initio computational study of the resonant Auger spectra of the HCl molecule close to the Cl L-II,L-III edge.

Keyword
VIBRATIONAL STRUCTURE, SYMMETRY-BREAKING, ELECTRONIC DECAY, HIGH-RESOLUTION, EMISSION SPECTRUM, SPECTROSCOPY, MOLECULES, APPROXIMATION, COLLAPSE, STATES
National Category
Atom and Molecular Physics and Optics Atom and Molecular Physics and Optics
Identifiers
urn:nbn:se:kth:diva-13834 (URN)000078778500034 ()
Note
QC 20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2017-12-12Bibliographically approved
3. Observation of a continuum-continuum interference hole in ultrafast dissociating core-excited molecules
Open this publication in new window or tab >>Observation of a continuum-continuum interference hole in ultrafast dissociating core-excited molecules
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2000 (English)In: Physical Review Letters, ISSN 0031-9007, E-ISSN 1079-7114, Vol. 85, no 15, 3133-3136 p.Article in journal (Refereed) Published
Abstract [en]

The femtosecond dissociation of HCl after core excitation has been studied through the resonant Auger decay. The spectra contain contributions from decay occurring at both "molecular" and "atomic" internuclear distances. We have observed a new interference mechanism in these spectra: An atomic spectral line develops into a negative spectral contribution, a "hole," when detuning the excitation energy from the maximum of the Cl 2p(-1)sigma* resonance. Resonant x-ray scattering theory quantitatively explains this behavior as due to a novel destructive continuum-Continuum interference between molecular and atomic contributions to the Auger decay.

Keyword
HCL, RAMAN, SCATTERING, EXCITATION, SPECTRA, STATES, DECAY, HBR
National Category
Physical Sciences
Identifiers
urn:nbn:se:kth:diva-13835 (URN)10.1063/1.1516805 (DOI)000089807800017 ()
Note
QC 20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2017-12-12Bibliographically approved
4. Dynamical suppression of atomic peaks in resonant dissociative photoemission
Open this publication in new window or tab >>Dynamical suppression of atomic peaks in resonant dissociative photoemission
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2001 (English)In: Chemical Physics Letters, ISSN 0009-2614, E-ISSN 1873-4448, Vol. 343, no 3-4, 332-338 p.Article in journal (Refereed) Published
Abstract [en]

Resonant excitation to the F1s-sigma* dissociative state in hydrogen fluoride gives a photoelectron spectrum where the spectator part contains strong atomic lines but a participator part where such lines are lacking. We demonstrate that this contrasting behaviour between the two parts is due to a strong dynamical suppression of the resonant contribution, making direct main state photoionization the dominating channel even at resonant conditions.

Keyword
ray raman-scattering, molecules, spectra, hcl, excitation, states, decay
National Category
Atom and Molecular Physics and Optics Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-13836 (URN)10.1016/S0009-2614(01)00667-4 (DOI)000170235700021 ()
Note
QC 20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2017-12-12Bibliographically approved
5. Theory and first principles calculations of dissociative resonant photoionization: The evolution of atomic peaks and holes
Open this publication in new window or tab >>Theory and first principles calculations of dissociative resonant photoionization: The evolution of atomic peaks and holes
2002 (English)In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 116, no 2, 629-645 p.Article in journal (Refereed) Published
Abstract [en]

We present theory and computational method for analyzing dissociative resonant photoemission from first principles. Particular emphasis is devoted to the conditions for observing so-called atomic peaks and atomic holes. The atomic peaks are connected with photoemission following resonant excitation to dissociative core excited states which show signals from scattering channels involving the dissociation (atomic) fragments in addition to those involving the compound molecule. The holes are the results of continuum-continuum interference effects between these two, atomic and molecular, channels which may act destructively under certain conditions. We apply a novel electronic structure method to compute the transition moments for the resonant and direct photoemission channels including their dependence on internuclear distances and their interference. The relevant matrix elements involving the photoelectron are obtained using similar techniques for the two types of channels, with the scattered electron wave in each case being determined in the full molecular anisotropic potential. A study of resonant photoemission through the core excited sigma* states of HF and HCl indicates that the appearance of the atomic peaks and holes is subtly dependent on the nuclear dynamics, the potential energy curves, and the excitation photon frequency. We demonstrate that the resonant contribution and the evolution of the atomic peaks can be subject to strong dynamical suppression, so strong in fact that main state photoionization may constitute the dominating channel even at resonant conditions. It is shown that such dynamical suppression explains that resonant excitation to the F 1s-sigma* dissociative state in hydrogen fluoride gives a photoelectron spectrum in which the spectator part contains strong atomic lines but a participator part where such lines are lacking, although they both refer to the same, dissociative, core excited state. The findings in the present work give evidence that both direct and resonant channels should be simultaneously considered in analyses of the dissociative photoemission process even at resonant conditions.

Keyword
RAY RAMAN-SCATTERING, AUGER SPECTRUM, CROSS-SECTIONS, DECAY, HCL, MOLECULES, PHOTOEMISSION, EXCITATION, INTERFERENCE, ELECTRON
National Category
Physical Sciences
Identifiers
urn:nbn:se:kth:diva-13837 (URN)10.1063/1.1423329 (DOI)000172926700019 ()
Note
QC 20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2017-12-12Bibliographically approved
6. Numerical implementation of a wave packet techniques in X-ray scattering
Open this publication in new window or tab >>Numerical implementation of a wave packet techniques in X-ray scattering
(English)Manuscript (preprint) (Other academic)
National Category
Natural Sciences
Identifiers
urn:nbn:se:kth:diva-13831 (URN)
Note
QC 20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2010-06-30Bibliographically approved
7. X-ray Raman scattering under pulsed excitation
Open this publication in new window or tab >>X-ray Raman scattering under pulsed excitation
2000 (English)In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 112, no 13, 5593-5603 p.Article in journal (Refereed) Published
Abstract [en]

Accounting for actual and anticipated developments in synchrotron radiation- and in x-ray and free electron laser techniques, we present a theory of resonant scattering of short-pulsed x rays. Both the instantaneous and integrated-over-observation-time x-ray scattering spectra are studied. Contrary to the commonly accepted notion of an instantaneous probability, we find that the correct quantity describing the resonant x-ray scattering (RXS) experiment is the probability integrated over the time of measurement. It is shown that the integral RXS probability is given by the convolution of the RXS probability for monochromatic excitation with the Wiener-Khintchine spectrum of the nonstationary incident radiation. We have found that short pulses yield a new spectral band following a non-Raman dispersion law. The finite duration of pulses results in a broadening of the Raman resonance. Some aspects of the theoretical analysis of the RXS spectra as functions of the pulse duration time are analyzed by numerical calculations.

Keyword
uger resonant raman, time, molecules, spectrum, light, model, co
National Category
Physical Sciences
Identifiers
urn:nbn:se:kth:diva-13838 (URN)10.1063/1.481134 (DOI)000085902300010 ()
Note
QC 20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2017-12-12Bibliographically approved
8. Doppler effects in resonant x-ray Raman scattering
Open this publication in new window or tab >>Doppler effects in resonant x-ray Raman scattering
1998 (English)In: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 57, no 4, 2511-2526 p.Article in journal (Refereed) Published
Abstract [en]

Theory for Doppler effects in resonant x-ray Raman scattering (RXS) is presented. It is shown that the "electron" Doppler effect is important in nonradiative RXS for decay transitions between continuum nuclear states lying above the dissociation threshold, and that the averaging of the RXS cross section over molecular orientations can lead to strong non-lorentzian broadenings of the atomiclike resonances. The Doppler effect is found to give a unique possibility to distinguish dissociating identical atoms, because different peaks correspond to atoms with opposite Doppler shifts. Spectral features of the atomiclike profile are predicted and analyzed. Strong oscillations of the RXS cross section will occur as a consequence of the interference of the Auger electrons. Due to the Doppler effect and the interference, the atomiclike profile can be associated with supernarrow spectral features, the width of which goes below the lifetime broadening and is practically independent of the spectral distribution of the incident radiation. As another consequence of the oscillations and strong anisotropy caused by the interference, we predict parity selection rules for Auger decay transitions in both bound and dissociative systems. The corresponding experiments can be realized by measurements of resonant Auger of surface adsorbed molecules and for molecules by the electron-ion coincidence technique.

Keyword
PHOTOELECTRON-SPECTROSCOPY, EMISSION-SPECTROSCOPY, ORIENTED MOLECULES, SPECTRA
National Category
Atom and Molecular Physics and Optics Physical Sciences
Identifiers
urn:nbn:se:kth:diva-13839 (URN)000073243700038 ()
Note
QC 20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2017-12-12Bibliographically approved
9. Generalized Franck-Condon principle for resonant photoemission
Open this publication in new window or tab >>Generalized Franck-Condon principle for resonant photoemission
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1999 (English)In: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 60, no 4, 2786-2791 p.Article in journal (Refereed) Published
Abstract [en]

A generalized Franck-Condon (GFC) principle for resonant x-ray Raman scattering and for resonant photoemission in particular is derived and numerically investigated. The GFC amplitudes differ from ordinary FC amplitudes by the presence of photon and photoelectron phase factors which describe the coupling-or interference-of the x-ray photons or Anger electrons with the nuclear motion. With the GFC amplitudes, a Kramers-Heisenberg relation is obtained for vibronic transitions that corrects the so-called lifetime-vibrational interference formula. For resonant photoemission in the soft-x-ray region involving typical bound potential surfaces, the generalization gives a contribution to the FC factors that can amount to 20%. For core excitation above the dissociation threshold, the GFC principle relates to Doppler effects on the ejected photoelectron both for the so-called "molecular'' and "atomic" bands. The role of the GFC principle in direct photoionization is briefly discussed.

Keyword
X-RAY-EMISSION, VIBRATIONAL STRUCTURE, AUGER, MOLECULES, SPECTRA, RAMAN, SPECTROSCOPY, STATES, DECAY, CO
National Category
Atom and Molecular Physics and Optics Physical Sciences
Identifiers
urn:nbn:se:kth:diva-13840 (URN)000083201000035 ()
Note
QC 20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2017-12-12Bibliographically approved
10. Doppler effect for bound nuclear motion and its manifestation in resonant photoemission of oriented systems
Open this publication in new window or tab >>Doppler effect for bound nuclear motion and its manifestation in resonant photoemission of oriented systems
2000 (English)In: Chemical Physics Letters, ISSN 0009-2614, E-ISSN 1873-4448, Vol. 328, no 4-6, 425-430 p.Article in journal (Refereed) Published
Abstract [en]

In contrast to the common notion that Doppler effects have relevance only for atoms or molecules in free motion, we show that such effects should clearly be observable - and accounted for - in resonant scattering also when the nuclei are in bound state quantized motion. This untrivial effect does not influence the position of single resonances but only the center of gravity of the spectra. It is found to strongly depend on the duration time of the scattering.

Keyword
RAY RAMAN-SCATTERING, CO MOLECULES, NACL(100), GRAPHITE, MIXTURES, DYNAMICS
National Category
Physical Sciences Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-13841 (URN)000089836500018 ()
Note
QC 20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2017-12-12Bibliographically approved
11. Vibrationally resolved core-photoelectron spectroscopy as an infinite-slit interferometry
Open this publication in new window or tab >>Vibrationally resolved core-photoelectron spectroscopy as an infinite-slit interferometry
2001 (English)In: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 64, no 1Article in journal (Refereed) Published
Abstract [en]

During a molecular vibration, an atom changes continuously its position. Just as the emitted photoelectron waves, the electromagnetic waves absorbed by the atom in the different positions are strictly coherent and have different well-defined phases. These phases depend on the relation between the instantaneous internuclear distance and the photoelectron, respectively, photon wavelengths. We predict that the interference of these coherent waves strongly influences the vibrational profile of the photoelectron spectra of core electrons in a molecule. This effect increases with increasing x-ray photon frequency and results in a deformation and broadening of the vibrational profile. In the case of surface adsorbed molecules, the vibrational profile depends strongly on the direction of the photoelectron ejection and photon momentum, and the orientational sensitivity of a vibrational profile can even be used as a tool to define the orientation of adsorbed molecules.

Keyword
RAY, PHOTOEMISSION, SCATTERING, MOLECULES
National Category
Atom and Molecular Physics and Optics Atom and Molecular Physics and Optics
Identifiers
urn:nbn:se:kth:diva-13848 (URN)000169711400040 ()
Note
QC 20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2017-12-12Bibliographically approved
12. Resonant x-ray Raman scattering involving avoided crossings in the final-state potential-energy curves
Open this publication in new window or tab >>Resonant x-ray Raman scattering involving avoided crossings in the final-state potential-energy curves
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2000 (English)In: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 62, no 6Article in journal (Refereed) Published
Abstract [en]

The role of avoided crossings for resonant x-ray Raman scattering is explored. The strong dependence of the electronic transition amplitudes on internuclear distance at avoided crossings causes new, and even anomalous, spectral features, and can bring about a breakdown of the generally accepted participator or spectator classification of the transitions. We report, and apply the theory on, an experimental observation of the electron decay of the N 1s-->pi* core-excited level in N-2 the B(2)Sigma (+)(u) final state with peculiar, non-Franck-Condon, vibrational intensity distributions.

Keyword
core-excited states, vibrational structure, carbon-monoxide, decay spectra, excitation, molecules, dynamics, n-2, photoemission, spectroscopy
National Category
Atom and Molecular Physics and Optics Atom and Molecular Physics and Optics
Identifiers
urn:nbn:se:kth:diva-13849 (URN)10.1016/s0009-2614(03)00681-x (DOI)000165697200037 ()
Note
QC 20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2017-12-12Bibliographically approved
13. Competition between decay and dissociation of core-excited carbonyl sulfide studied by x-ray scattering
Open this publication in new window or tab >>Competition between decay and dissociation of core-excited carbonyl sulfide studied by x-ray scattering
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1999 (English)In: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 59, no 6, 4281-4287 p.Article in journal (Refereed) Published
Abstract [en]

We show evidence of dissociation during resonant inelastic soft x-ray scattering Carbon and oxygen K-shell and sulfur L-shell resonant and nonresonant x-ray emission spectra were measured using monochromatic synchrotron radiation for excitation and ionization. After sulfur L-2,L-3-->pi*, sigma* excitation, atomic lines are observed in the emission spectra as a consequence of competition between de-excitation and dissociation. In contrast thr carbon and oxygen spectra show weaker line-shape variations and no atomic Lines. The spectra are compared to results from ab initio calculations. The discussion of the dissociation paths is based on calculated potential energy surfaces and atomic transition energies.

Keyword
HIGH-RESOLUTION, OCS MOLECULE, ABSORPTION SPECTRA, STATIC EXCHANGE, AUGER-SPECTRA, AB-INITIO, EMISSION, CS2, DYNAMICS, HCL
National Category
Atom and Molecular Physics and Optics Atom and Molecular Physics and Optics
Identifiers
urn:nbn:se:kth:diva-13850 (URN)000080777600024 ()
Note
QC 20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2017-12-12Bibliographically approved
14. Picturing molecular femtosecond processes through an ultra-fast controllable X-ray shutter
Open this publication in new window or tab >>Picturing molecular femtosecond processes through an ultra-fast controllable X-ray shutter
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2003 (English)In: Chemical Physics, ISSN 0301-0104, E-ISSN 1873-4421, Vol. 289, no 1, 51-56 p.Article in journal (Refereed) Published
Abstract [en]

We show that frequency detuning in a resonant X-ray scattering experiment acts as an X-ray camera shutter by regulating the duration time of the scattering process. The camera shutter can be used to select processes at different time scales for observation. This is illustrated by a resonant Auger study of the ultra-fast dissociation of the core-excited HF molecule. We present experimental results and first principle simulations of the molecular fraction in the resonant Auger spectra of HF which is a dynamical parameter that well illustrates X-ray shutter controlled dissociation.

Keyword
RAMAN-SCATTERING, VIBRATIONAL STRUCTURE, SYMMETRY-BREAKING, ATOMIC PEAKS, EXCITATION, SPECTRA, HCL, SPECTROSCOPY, DISSOCIATION, HF
National Category
Physical Chemistry Atom and Molecular Physics and Optics
Identifiers
urn:nbn:se:kth:diva-13851 (URN)10.1016/S0301-0104(02)00796-6 (DOI)000181788600006 ()
Note
QC 20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2017-12-12Bibliographically approved
15. Dynamics of Inner Shell Resonant Raman Scattering.
Open this publication in new window or tab >>Dynamics of Inner Shell Resonant Raman Scattering.
1999 (English)In: Journal of the Japanese Society for Synchrotron Radiation Research, ISSN 0914-9287, Vol. 12, no 4, 257-267 p.Article in journal (Refereed) Published
Abstract [en]

Some recent advances in the theory of the resonant Raman process for atoms, molecules and solids involving inner shell electrons are reviewed. Special emphasis is put on the dynamical aspects and on the notion of a duration time for the x-ray Raman process (RXS), which brings about a distinetion of processes with different time scales responsible for the formation of the spectral profile. This notion has been useful for actual predietions of various phenomena associated with RXS such as "symmetry restoration" "vibrational collapse", and "control of dissociation". The temporal theory of RXS is based on the wave packet formalism. The increase of the broad "molecular" parts relative to the atomic, or fragment, decay upon frequency detuning is demonstrated. The atomic-like resonance and molecular parts are proved to show different dispersion relations. Under certain conditions the interference between the molecular and atomic parts produces conspicuous "spectral holes". These conceptual tools are applicable also in the case of solids; there is an analogous restoration of momentum selection rules and a collapse effect upon detuning the frequency. Thus when the duration of the scattering is shortened by a large detuning, the role of electron-phonon coupling of the core excited states is suppresssed. The shortening of the RXS duration in a certain sense leads to a deloealization of the core hole in a solid. We describe also some new features that derive from the Doppler effect on ejected Auger electrons.

National Category
Natural Sciences
Identifiers
urn:nbn:se:kth:diva-13847 (URN)
Note
QC 20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2010-06-30Bibliographically approved

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