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Spin-Orbit Coupling and Metal-Ligand Interactions in Fe(II), Ru(II), and Os(II) Complexes
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Surface and Interface Science.
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Surface and Interface Science.
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2010 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 114, no 22, 10314-10322 p.Article in journal (Refereed) Published
Abstract [en]

The purpose of the present paper is to experimentally map the energy levels governing the trends observed in oxidation potentials and absorption spectra of M(bpy)(3)(2+) complexes (bpy = 2,2'-bipyridine, M = Fe(II), Ru(II), and Os(II)). Molecular films of the transition metal complexes were investigated with element specific methods using photoelectron spectroscopy (PES) at high kinetic energy using hard X-rays and by X-ray absorption spectroscopy (XAS). The results were compared to electronic structure calculations on the complexes and the ligand. The approach allows us to experimentally measure and interpret the energy levels in terms of spin orbit coupling and metal ligand interactions. Specifically, it was verified that the anomaly in the trend in oxidation potentials could be explained by a large spin orbit coupling for the Os(bpy)(3)(2+). The influence of the different metal ions on the state formed upon light absorption was also investigated by N Is X-ray absorption, and from the spectra we could determine the relative position of the levels originating from d-sigma and pi contributions. The results for the occupied and unoccupied electronic levels explain the lower energy of the MLCT transition of the Os(bpy)(3)(2+) in comparison to the Ru(bpy)(3)(2+).

Place, publisher, year, edition, pages
2010. Vol. 114, no 22, 10314-10322 p.
National Category
Physical Sciences
URN: urn:nbn:se:uu:diva-136087DOI: 10.1021/jp103884cISI: 000278301200032OAI: oai:DiVA.org:uu-136087DiVA: diva2:376185
Available from: 2010-12-10 Created: 2010-12-09 Last updated: 2016-04-20Bibliographically approved
In thesis
1. Techniques and Application of Electron Spectroscopy Based on Novel X-ray Sources
Open this publication in new window or tab >>Techniques and Application of Electron Spectroscopy Based on Novel X-ray Sources
2012 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The curiosity of researchers to find novel characteristics and properties of matter constantly pushes for the development of instrumentation based on X-radiation. I present in this thesis techniques for electron spectroscopy based on developments of X-ray sources both in time structure and energy. One part describes a laser driven High-Harmonic Generation source and the application of an off-plane grating monochromator with additional beamlines and spectrometers. In initial experiments, the source is capable of producing harmonics between the 13th and 23rd of the fundamental laser 800 nm wavelength. The intensity in the 19th harmonic, after monochromatization, was measured to be above 1.2·1010 photons/second with a repetition rate of 5 kHz. 

The development of a chopper system synchronized to the bunch clock of an electron storage ring is also presented. The system can be used to adjust the repetition rate of a synchrotron radiation beam to values between 10 and 120 kHz, or for the modulation of continuous sources. The application of the system to both time of flight spectroscopy and laser pump X-ray probe spectroscopy is shown. It was possible to measure triple ionization of Kr and in applied studies the valence band of a laser excited dye-sensitized solar cell interface. The combination of the latter technique with transient absorption measurements is proposed.

The organic molecule maleic anhydride (MA) and its binding configuration to the three anatase TiO2 crystals (101), (100), (001) has been investigated by means of Xray Photoelectron Spectroscopy (XPS) and Near Edge X-ray Absorption Fine structure Spectroscopy (NEXAFS). The results provide information on the binding configuration to the 101 crystal. High Kinetic Energy Photoelectron Spectroscopy was used to investigate multilayers of complexes of iron, ruthenium and osmium. The benefit of hard X-rays for ex-situ prepared samples is demonstrated together with the application of resonant valence band measurements to these molecules.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2012. 53 p.
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 903
High Harmonic Generation HHG, HELIOS, X-ray Beam Chopper, Dye-sensitized Solar Cell, Ultra High Vacuum UHV, Photoelectron Spectroscopy, Pump-Probe, XUV
National Category
Physical Sciences
Research subject
Physics with spec. in Atomic, Molecular and Condensed Matter Physics
urn:nbn:se:uu:diva-168799 (URN)978-91-554-8283-1 (ISBN)
Public defence
2012-03-30, Pol/1311, Polacksbacken, Lägerhyddsvägen 2, Uppsala, 10:15 (English)
Available from: 2012-03-09 Created: 2012-02-15 Last updated: 2012-09-18Bibliographically approved

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Rensmo, Håkan
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