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Electronic structure studies using resonant X-ray and photoemission spectroscopy
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics.
1999 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This thesis addresses the electronic structure of molecules and solids using resonant X-ray emission and photoemission spectroscopy. The use of monochromatic synchrotron radiation and the improved performance of the instrumentation have opened up the possibility of detailed analyses of the response of the electronic systems under interaction with X-rays. The experimental studies are accompanied by numerical ab initio calculations in the formalism of resonant inelastic scattering. The energy selectivity has made it possible for the first time to study how the chemical bonds in a molecule break up during resonant inelastic X-ray scattering. In the conjugated polymer systems, the element selectivity of the X-ray emission process made it possible to probe the different atomic elements separately. The X-ray emission technique proved to be useful for extracting isomeric information, and for measuring the change in the valence levels at different degrees of doping. In this thesis, spectral satellite features in transition metals were thoroughly investigated for various excitation energies around a core-level threshold. By measuring the relative spectral intensity of the satellites it was possible to extract information on the partial core-level widths. Using the nickel metal system as an example, it was shown that it is possible to probe the different core-excited states close toshake-up thresholds by measuring the relative spectral intensity variation of the Auger emission.Resonant photoemission measurements showed unambiguous evidence of interference effects. Theseeffects were also thoroughly probed using angle-dependent measurements. The combination of X-rayemission and absorption were useful for studying buried layers and interfaces due to the appreciable penetration depth of soft X-rays. X-ray scattering was further found to be useful for studying low-energy excited states of rare earth metallic compounds and transition metal oxides.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis , 1999. , p. 95
Series
Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1104-232X ; 452
Keywords [en]
Physics
Keywords [sv]
Fysik
National Category
Physical Sciences
Research subject
Physics
Identifiers
URN: urn:nbn:se:uu:diva-973ISBN: 91-554-4463-6 (print)OAI: oai:DiVA.org:uu-973DiVA, id: diva2:173311
Public defence
1999-05-14, Siegbahn Lecture hall, Department of Physics, Uppsala University, Uppsala, 10:00
Available from: 1999-04-23 Created: 1999-04-23 Last updated: 2013-10-10Bibliographically approved
List of papers
1. 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, p. 4281-4287Article 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 L2,3→π*, σ* excitation, atomic lines are observed in the emission spectra as a consequence of competition between de-excitation and dissociation. In contrast the 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.

Keywords
HIGH-RESOLUTION; OCS MOLECULE; ABSORPTION SPECTRA; STATIC EXCHANGE; AUGER-SPECTRA; AB-INITIO; EMISSION; CS2; DYNAMICS; HCL
National Category
Physical Sciences
Identifiers
urn:nbn:se:uu:diva-67148 (URN)10.1103/PhysRevA.59.4281 (DOI)
Available from: 2006-11-08 Created: 2006-11-08 Last updated: 2017-11-28Bibliographically approved
2. Resonant and nonresonant x-ray scattering spectra of some poly(phenylenevinylene)s
Open this publication in new window or tab >>Resonant and nonresonant x-ray scattering spectra of some poly(phenylenevinylene)s
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1998 (English)In: JOURNAL OF CHEMICAL PHYSICS, ISSN 0021-9606, Vol. 108, no 14, p. 5990-5996Article in journal (Other scientific) Published
Abstract [en]

The electronic structure of some poly(phenylenevinylene)s have been investigated by resonant and nonresonant x-ray inelastic scattering spectroscopies. The nonresonant as well as all resonant spectra for each polymer demonstrate benzene-like features, ind

Keywords
FLUORESCENCE; MOLECULES; EMISSION; INTERFERENCE; EXCITATION; ANISOTROPY; POLYMERS; GRAPHITE; DIODES
Identifiers
urn:nbn:se:uu:diva-71287 (URN)
Note
Addresses: Guo JH, Univ Uppsala, Dept Phys, Box 530, S-75121 Uppsala, Sweden. Univ Uppsala, Dept Phys, S-75121 Uppsala, Sweden. Linkoping Univ, Inst Phys & Measurement Technol, S-58183 Linkoping, Sweden. Univ Durham, IRC Polymer Sci & Technol, Durham DH1Available from: 2006-11-08 Created: 2006-11-08 Last updated: 2013-10-10
3. The electronic structure of poly(pyridine-2,5-diyl) investigated by soft X-ray absorption and emission spectroscopies
Open this publication in new window or tab >>The electronic structure of poly(pyridine-2,5-diyl) investigated by soft X-ray absorption and emission spectroscopies
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1998 (English)In: Chemical Physics, ISSN 0301-0104, E-ISSN 1873-4421, Vol. 237, no 3, p. 295-304Article in journal (Refereed) Published
Abstract [en]

The electronic structure of the poly-pyridine conjugated polymer has been investigated by resonant and non-resonant inelastic X-ray scattering and X-ray absorption spectroscopies using synchrotron radiation. The measurements were made for both the carbon and nitrogen contents of the polymer. The analysis of the spectra has been carried out in comparison with molecular orbital calculations taking the repeat-unit cell as a model molecule of the polymer chain. The simulations indicate no significant differences in the absorption and in the non-resonant X-ray scattering spectra for the different isomeric geometries, while some isomeric dependence of the resonant spectra is predicted. The resonant emission spectra show depletion of the π electron bands in line with symmetry selection and momentum conservation rules. The effect is most visual for the carbon spectra; the nitrogen spectra are dominated by lone pair n orbital emission of σ symmetry and are less frequency dependent.

Keywords
STATIC-EXCHANGE CALCULATIONS; SPECTRA; MOLECULES; EXCITATION; POLY(2;2'-BIPYRIDINE-5;5'-DIYL); POLY(P-PYRIDINE); INTERFERENCE; FLUORESCENCE; SCATTERING; POLYMERS
National Category
Physical Sciences
Identifiers
urn:nbn:se:uu:diva-70298 (URN)10.1016/S0301-0104(98)00262-6 (DOI)
Available from: 2006-11-09 Created: 2006-11-09 Last updated: 2017-11-21Bibliographically approved
4. Resonant inelastic soft X-ray scattering spectra at the nitrogen and carbon K-edges of poly(pyridine-2,5-diyl)
Open this publication in new window or tab >>Resonant inelastic soft X-ray scattering spectra at the nitrogen and carbon K-edges of poly(pyridine-2,5-diyl)
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1999 (English)In: Journal of Electron Spectroscopy and Related Phenomena, ISSN 0368-2048, E-ISSN 1873-2526, Vol. 101-103, p. 573-578Article in journal (Refereed) Published
Abstract [en]

Resonant inelastic scattering measurements of the conjugated polymer, poly(pyridine-2,5-diyl) have been performed at the nitrogen and carbon K-edges using synchrotron radiation. For comparison, molecular orbital calculations of the spectra have been carried out with the repeat unit as a model molecule of the polymer chain. The resonant emission spectra show depletion of the π electron bands which is consistent with symmetry selection and momentum conservation rules. The depletion is most obvious in the resonant inelastic scattering spectra of carbon while the nitrogen spectra are dominated by lone pair n orbital emission of σ symmetry and are less excitation energy dependent. By comparing the measurements to calculations an isomeric dependence of the resonant spectra is found giving preference to two of the four possible isomers in the polymer.

Keywords
resonant soft X-ray emission; X-ray scattering; conjugated polymers; CONJUGATED POLYMERS; RAMAN-SCATTERING; DOPED STATES; POLY(2;2'-BIPYRIDINE-5;5'-DIYL); POLY(P-PYRIDINE); SPECTROSCOPY
National Category
Physical Sciences
Identifiers
urn:nbn:se:uu:diva-67042 (URN)10.1016/S0368-2048(98)00354-5 (DOI)
Available from: 2006-11-15 Created: 2006-11-15 Last updated: 2017-11-28Bibliographically approved
5. The electronic structure of polyaniline and doped phases studied by soft x-ray absorption and emission spectroscopies
Open this publication in new window or tab >>The electronic structure of polyaniline and doped phases studied by soft x-ray absorption and emission spectroscopies
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1999 (English)In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 111, no 10, p. 4756-4761Article in journal (Refereed) Published
Abstract [en]

The electronic structure of the conjugated polymer, polyaniline, has been studied by resonant and nonresonant soft x-ray emission spectroscopy using synchrotron radiation for the excitation. The measurements were made on polyaniline and a few doped (protonated) phases for both the carbon and nitrogen contents. The resonant x-ray emission spectra show depletion of the π electron bands due to the selective excitation which enhances the effect of symmetry selection rules. The valence band structures in the x-ray emission spectra attributed to the π bands show unambiguous changes of the electronic structure upon protonation. By comparing to x-ray absorption measurements, the chemical bonding and electronic configuration is characterized.

Keywords
ELECTRICAL-CONDUCTIVITY; SCATTERING SPECTRA; POLYMERS; EDGE; FLUORESCENCE; POLYPYRROLE; DERIVATIVES; EXCITATION; RESONANCE; NITROGEN
National Category
Physical Sciences
Identifiers
urn:nbn:se:uu:diva-66706 (URN)10.1063/1.479238 (DOI)
Available from: 2006-11-08 Created: 2006-11-08 Last updated: 2017-11-28Bibliographically approved
6. Energy dependence of Cu L2,3 satellites using synchrotron excited x-ray-emission spectroscopy
Open this publication in new window or tab >>Energy dependence of Cu L2,3 satellites using synchrotron excited x-ray-emission spectroscopy
1997 (English)In: Physical Review B Condensed Matter, ISSN 0163-1829, E-ISSN 1095-3795, Vol. 56, no 19, p. 12238-12242Article in journal (Refereed) Published
Abstract [en]

The L2,3 x-ray emission of Cu metal has been measured using monochromatic synchrotron radiation. The self-absorption effect in the spectra is shown to be very small in our experimental geometry. From the quantitative analysis of spectra recorded at different excitation energies, the L3/L2 emission intensity ratio and the partial Auger width are extracted. High-energy satellite features on the L3 emission line are separated by a subtraction procedure. The satellite intensity is found to be slowly increasing for excitation energies between the L3, L2, and L1 core-level thresholds due to shake-up and shake-off transitions. As the excitation energy passes the L2 threshold, a step of rapidly increasing satellite intensity of the L3 emission is found due to additional Coster-Kronig processes.

Keywords
2P-X-RAY PHOTOELECTRON SPECTROSCOPIES; COSTER-KRONIG PROCESS; AUGER-SPECTRA; SOLID-STATE; FLUORESCENCE; COPPER; ZN; RADIATION; 2P
National Category
Physical Sciences
Identifiers
urn:nbn:se:uu:diva-72128 (URN)10.1103/PhysRevB.56.12238 (DOI)
Available from: 2006-11-15 Created: 2006-11-15 Last updated: 2017-12-14Bibliographically approved
7. Resonant Auger spectroscopy at the L2,3 shake-up thresholds as a probe of electron correlation effects in nickel
Open this publication in new window or tab >>Resonant Auger spectroscopy at the L2,3 shake-up thresholds as a probe of electron correlation effects in nickel
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1998 (English)In: Physical Review B Condensed Matter, ISSN 0163-1829, E-ISSN 1095-3795, Vol. 58, no 7, p. 3677-3681Article in journal (Refereed) Published
Abstract [en]

The excitation energy dependence of the three-hole satellites in the L3-M45M45 andL2-M45M45 Auger spectra of nickel metal has been measured using synchrotron radiation. The satellite behavior in the nonradiative emission spectra at the L3 and L2thresholds is compared and the influence of the Coster-Kronig channel explored. The three-hole satellite intensity at the L3 Auger emission line reveals a peak structure at 5 eV above the L3 threshold attributed to resonant processes at the 2p53d9 shake-up threshold. This is discussed in connection with the 6-eV feature in the x-ray-absorption spectrum.

Keywords
X-RAY-ABSORPTION; MAGNETIC-CIRCULAR-DICHROISM; NI VALENCE-BAND; FERROMAGNETIC NICKEL; TRANSITION-METALS; SELF-ENERGY; CORE-LEVEL; PHOTOEMISSION; SPECTRA; COPPER
National Category
Physical Sciences
Identifiers
urn:nbn:se:uu:diva-70591 (URN)10.1103/PhysRevB.58.3677 (DOI)
Available from: 2006-11-09 Created: 2006-11-09 Last updated: 2017-11-21Bibliographically approved
8. Resonant photoemission at the 2p edges of Ni: Resonant Raman and interference effects
Open this publication in new window or tab >>Resonant photoemission at the 2p edges of Ni: Resonant Raman and interference effects
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1997 (English)In: PHYSICAL REVIEW LETTERS, ISSN 0031-9007, Vol. 78, no 5, p. 967-970Article in journal (Other scientific) Published
Abstract [en]

Unambiguous evidence for resonant photoemission in Ni is presented. Interference effects are identified at the 2p edges for the valence band and the 6 eV satellite. A rapid transition from a resonant Raman to an Auger-like regime shows that the core-excit

Keywords
VALENCE-BAND PHOTOEMISSION; AUGER-SPECTRA; NICKEL
Identifiers
urn:nbn:se:uu:diva-73912 (URN)
Note
Addresses: Weinelt M, UNIV UPPSALA, DEPT PHYS, BOX 530, S-75121 UPPSALA, SWEDEN. IBM CORP, ALMADEN RES CTR, DIV RES, SAN JOSE, CA 95120.Available from: 2006-11-09 Created: 2006-11-09 Last updated: 2013-10-10
9. Angular-dependent resonant-photoemission processes at the 2p thresholds in nickel metal
Open this publication in new window or tab >>Angular-dependent resonant-photoemission processes at the 2p thresholds in nickel metal
1999 (English)In: Physical Review B Condensed Matter, ISSN 0163-1829, E-ISSN 1095-3795, Vol. 60, no 4, p. 2436-2440Article in journal (Refereed) Published
Abstract [en]

Angle-resolved valence-band resonant-photoemission of nickel metal has been measured close to the 2p core-level thresholds with synchrotron radiation. The well-known 6-eV correlation satellite has an intensity enhancement of about two orders of magnitude at resonance. The angular dependence of the photoemission intensity has been studied as function of photon energy and provides unambiguous evidence for interference effects all the way up to the resonance maximum. The observation of different angular asymmetries, β, for the valence band and the satellite is discussed in connection to the origin of the resonant-photoemission process and the character of the satellite.  

Keywords
KRONIG AUGER DECAY; VALENCE-BAND PHOTOEMISSION; LIII THRESHOLDS; NI METAL; CORE-LEVEL; CUO; SPECTRA; INTERFERENCE; SPLITTINGS; SATELLITE
National Category
Physical Sciences
Identifiers
urn:nbn:se:uu:diva-66848 (URN)10.1103/PhysRevB.60.2436 (DOI)
Available from: 2006-11-09 Created: 2006-11-09 Last updated: 2017-11-28Bibliographically approved
10. Coherent and incoherent processes in resonant photoemission
Open this publication in new window or tab >>Coherent and incoherent processes in resonant photoemission
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1997 (English)In: APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING, ISSN 0947-8396, Vol. 65, no 2, p. 159-167Article in journal (Other scientific) Published
Abstract [en]

The basis for resonant photoemission is discussed in connection with data for a physisorption system, Ar/Pt(111) and a 3d transition metal, Ni(100). For Ar/Pt(111) the quasi-localized character of the intermediate state leads to two types of features in t

Keywords
AUGER-SPECTRA; NI METAL; FLUORESCENCE; TRANSITIONS; EXCITATION; THRESHOLDS; DECAY
Identifiers
urn:nbn:se:uu:diva-72898 (URN)
Note
Addresses: Martensson N, UNIV UPPSALA, DEPT PHYS, BOX 530, S-75121 UPPSALA, SWEDEN. IBM CORP, ALMADEN RES CTR, DIV RES, SAN JOSE, CA 95120.Available from: 2006-11-09 Created: 2006-11-09 Last updated: 2013-10-10
11. X-ray fluorescence spectra of metals excited below threshold
Open this publication in new window or tab >>X-ray fluorescence spectra of metals excited below threshold
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2003 (English)In: Physical Review B Condensed Matter, ISSN 0163-1829, E-ISSN 1095-3795, Vol. 68, no 4, p. 045119-Article in journal (Refereed) Published
Abstract [en]

X-ray scattering spectra of Cu and Ni metals have been measured using monochromatic synchrotron radiation tuned from far above to more than 10 eV below threshold. Energy conservation in the scattering process is found to be sufficient to explain the modulation of the spectral shape, neglecting momentum conservation and channel interference. At excitation energies close to and above threshold, the emission spectra map the occupied local partial density of states. For the subthreshold excitations, the high-energy flank of the inelastic scattering exhibits a Raman-type linear dispersion, and an asymmetric low-energy tail develops. For excitation far below threshold the emission spectra are proportional to a convolution of the occupied and unoccupied local partial densities of states.

National Category
Physical Sciences
Identifiers
urn:nbn:se:uu:diva-25528 (URN)10.1103/PhysRevB.68.045119 (DOI)
Available from: 2007-02-13 Created: 2007-02-13 Last updated: 2017-12-07Bibliographically approved
12. ELECTRONIC-STRUCTURE OF BURIED SI LAYERS IN GAAS(001) AS STUDIED BY SOFT-X-RAY EMISSION
Open this publication in new window or tab >>ELECTRONIC-STRUCTURE OF BURIED SI LAYERS IN GAAS(001) AS STUDIED BY SOFT-X-RAY EMISSION
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1995 (English)In: Physical Review B-CONDENSED MATTER, Vol. 52, p. R8643-Article in journal (Refereed) Published
Abstract [en]

It is demonstrated that it is possible to investigate details of the electronic structure of an internal atomic monolayer using soft-x-ray-emission spectroscopy. The local and partial density of states of one monolayer and three monolayers of Si, embedded

Keywords
SPECTROSCOPY; DENSITIES; SPECTRA; STATES; GAAS
Identifiers
urn:nbn:se:uu:diva-75824 (URN)
Note
Addresses: NILSSON PO, CHALMERS UNIV TECHNOL, DEPT PHYS, S-41296 GOTHENBURG, SWEDEN. UNIV UPPSALA, DEPT PHYS, S-75121 UPPSALA, SWEDEN.Available from: 2006-11-15 Created: 2006-11-15 Last updated: 2013-10-10
13. Electronic structure of Cu/Ni(100) interfaces
Open this publication in new window or tab >>Electronic structure of Cu/Ni(100) interfaces
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(English)Manuscript (preprint) (Other academic)
National Category
Natural Sciences
Identifiers
urn:nbn:se:uu:diva-208902 (URN)
Available from: 2013-10-10 Created: 2013-10-10 Last updated: 2013-10-10Bibliographically approved
14. Resonant inelastic soft-X-ray scattering at the 4d edge of Ce-based heavy-fermion materials
Open this publication in new window or tab >>Resonant inelastic soft-X-ray scattering at the 4d edge of Ce-based heavy-fermion materials
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1999 (English)In: JOURNAL OF ELECTRON SPECTROSCOPY AND RELATED PHENOMENA, ISSN 0368-2048, Vol. 103, p. 783-786Article in journal (Other scientific) Published
Abstract [en]

Resonant X-ray scattering measurements were performed on CeB6, CeAl, gamma-Ce, and alpha-Ce at various incident-photon energies near the Ce 4d threshold. A pronounced inelastic scattering structure which has 4f character is observed at about 4 eV below th

Keywords
Resonant soft-X-ray scattering; Ce-based heavy-fermion systems; charge-transfer excitations; X-ray absorption; SPECTROSCOPY; EXCITATIONS; MODEL
Identifiers
urn:nbn:se:uu:diva-67073 (URN)
Note
Addresses: Butorin SM, Univ Uppsala, Dept Phys, Box 530, S-75121 Uppsala, Sweden. Univ Uppsala, Dept Phys, S-75121 Uppsala, Sweden. Lawrence Berkeley Lab, Div Chem Sci, Berkeley, CA 94720 USA. Tohoku Univ, Dept Phys, Sendai, Miyagi 98077, Japan.Available from: 2006-11-08 Created: 2006-11-08 Last updated: 2013-10-10
15. Soft X-ray scattering from CeBat the 3d and 4d thresholds
Open this publication in new window or tab >>Soft X-ray scattering from CeBat the 3d and 4d thresholds
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(English)Manuscript (preprint) (Other academic)
National Category
Natural Sciences
Identifiers
urn:nbn:se:uu:diva-208906 (URN)
Available from: 2013-10-10 Created: 2013-10-10 Last updated: 2013-10-10Bibliographically approved
16. Resonant inelastic soft-x-ray scattering from valence-band excitations in 3d(0) compounds
Open this publication in new window or tab >>Resonant inelastic soft-x-ray scattering from valence-band excitations in 3d(0) compounds
1997 (English)In: PHYSICAL REVIEW B-CONDENSED MATTER, ISSN 0163-1829, Vol. 55, no 7, p. 4242-4249Article in journal (Other scientific) Published
Abstract [en]

Ti and Mn L(alpha,beta) x-ray fluorescence spectra of FeTiO3 and KMnO4 were measured with monochromatic photon excitation on selected energies across the L(2,3) absorption edges. The resulting inelastic x-ray-scattering structures and their changes with v

Keywords
ELECTRONIC-STRUCTURE; ANDERSON MODEL; PHOTOEMISSION; SPECTRA; SPECTROSCOPY; SATELLITES; OXIDES; EDGES; HYBRIDIZATION; TRANSITIONS
Identifiers
urn:nbn:se:uu:diva-73764 (URN)
Note
Addresses: Butorin SM, LINKOPING UNIV, DEPT PHYS & MEASUREMENTS TECHNOL, S-58183 LINKOPING, SWEDEN. UNIV UPPSALA, DEPT PHYS, S-75121 UPPSALA, SWEDEN. LUND UNIV, MAX LAB, S-22100 LUND, SWEDEN.Available from: 2006-11-08 Created: 2006-11-08 Last updated: 2013-10-10
17. Low-energy d-d excitations in MnO studied by resonant x-ray fluorescence spectroscopy
Open this publication in new window or tab >>Low-energy d-d excitations in MnO studied by resonant x-ray fluorescence spectroscopy
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1996 (English)In: PHYSICAL REVIEW B-CONDENSED MATTER, ISSN 0163-1829, Vol. 54, no 7, p. 4405-4408Article in journal (Other scientific) Published
Abstract [en]

We measured the Mn L(alpha,beta) x-ray fluorescence spectra of MnO excited by selected photon energies near the L(2,3) absorption edges. The resulting resonant inelastic x-ray scattering spectra probe low-lying electronic excited states, due to dd and cha

Keywords
ANDERSON MODEL; ABSORPTION-SPECTROSCOPY; SCATTERING; DICHROISM; SYMMETRY; METALS; EDGE
Identifiers
urn:nbn:se:uu:diva-74611 (URN)
Note
Addresses: UNIV UPPSALA, DEPT PHYS, S-75121 UPPSALA, SWEDEN.Available from: 2006-11-08 Created: 2006-11-08 Last updated: 2013-10-10

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