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Role of electron-phonon interaction in resonant x-ray Raman scattering by polymers and solids
KTH, Superseded Departments, Biotechnology.
KTH, Superseded Departments, Biotechnology.ORCID iD: 0000-0002-1763-9383
1999 (English)In: Physical Review B. Condensed Matter and Materials Physics, ISSN 1098-0121, E-ISSN 1550-235X, Vol. 59, no 14, 9243-9258 p.Article in journal (Refereed) Published
Abstract [en]

We present a theory of radiative resonant x-ray Raman scattering by solids and polymers beyond the Born-Oppenheimer approximation. The role of electron-phonon coupling of the intermediate core excited and final electronic states is analyzed in detail for π-electron systems and solids assuming the frozen-orbital approximation. The momentum exchange processes between valence electrons and phonons and with x-ray photons are analyzed, showing the similarities and differences between the two processes. The resonant inelastic x-ray scattering by a π-electron system is quenched up to zero in the Born-Oppenheimer approximation with frozen orbitals if the momentum exchange between valence electrons and x-ray photons is neglected. The electron-phonon and electron-photon interactions open the scattering channels for all occupied states in π systems. The frequency dependence of these effects is analyzed, showing that when the duration of the scattering is shortened by a large detuning of the excitation frequency, the role of electron-phonon coupling of both core-excited and final states is suppressed, depleting the cross section for π systems up to zero. The detuning quenches the symmetry breaking of the core-excited electronic states and results in a restoration of the selection rules and a conservation of electron momentum. Specific selection rules for the zero-phonon line in x-ray Raman spectra of linear polyenes are found. A detailed investigation of the narrowing, or collapse, of the electron-vibrational bands is given. When the detuning is large, the spectral profile is described by a joint density of states. It is predicted that the singularities of this joint density of states follows the Raman-Stokes dispersion law, something that allows a mapping of the band structure. We found that the phonon broadening of these singularities is completely quenched by detuning. A detailed investigation of the spectral shape versus detuning of the so-called excitonic band is given.

Place, publisher, year, edition, pages
1999. Vol. 59, no 14, 9243-9258 p.
National Category
Natural Sciences
Identifiers
URN: urn:nbn:se:kth:diva-13609DOI: 10.1103/PhysRevB.59.9243OAI: oai:DiVA.org:kth-13609DiVA: diva2:326180
Note
QC 20100622Available from: 2010-06-22 Created: 2010-06-22 Last updated: 2010-06-29Bibliographically approved
In thesis
1. X-ray scattering by molecules, surface-adsorbates and solids with a coupling to the nuclear motion
Open this publication in new window or tab >>X-ray scattering by molecules, surface-adsorbates and solids with a coupling to the nuclear motion
2000 (English)Licentiate thesis, comprehensive summary (Other scientific)
Place, publisher, year, edition, pages
Stockholm: KTH, 2000. vi, 36 p.
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-1120 (URN)91-7170-556-2 (ISBN)
Note
QC 20100622Available from: 2000-09-26 Created: 2000-09-26 Last updated: 2010-06-22Bibliographically approved
2. Electronic and nuclear dynamics of X-ray processes
Open this publication in new window or tab >>Electronic and nuclear dynamics of X-ray processes
2001 (English)Doctoral thesis, comprehensive summary (Other scientific)
Place, publisher, year, edition, pages
Stockholm: KTH, 2001. viii, 68 p.
Keyword
resonant X-ray Raman scattering, nuclear dynamics, relaxation
National Category
Industrial Biotechnology
Identifiers
urn:nbn:se:kth:diva-3189 (URN)91-7283-095-6 (ISBN)
Public defence
2001-06-12, 00:00
Note
QC 20100628Available from: 2001-06-08 Created: 2001-06-08 Last updated: 2010-06-29Bibliographically approved

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