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Adatoms, Quasiparticles & Photons: The Multifaceted World of Photoelectron Spectroscopy
KTH, School of Information and Communication Technology (ICT), Microelectronics and Applied Physics, MAP.ORCID iD: 0000-0002-3086-9642
2007 (English)Doctoral thesis, comprehensive summary (Other scientific)
Abstract [en]

The experimental work presented in this thesis is based on a wide assortment of very advanced and highly sophisticated photoelectron spectroscopy (PES) techniques. The objective of the present study has been to reveal and understand the electronic structure and electron dynamics in a broad spectrum of materials, ranging from wide band gap oxides, via semiconductors along with metals, and finally high-temperature superconductors.

The first part of the thesis concerns laser-based pump-and-probe PES. This unique experimental technique has permitted a study of the excited electronic structure and the electron dynamics of several semiconductor surfaces. An insight into details of the adatom to restatom charge-transfer of the Ge(111)c(2x8) surface is presented, as well as an estimate for the timescale in which the dynamic adatoms of the Ge(111):Sn(sqrt3xsqrt3)R30deg surface operate. Further results comprise a novel unoccupied surface state at the GaSb(001) surface as well as a time-resolved study of the charge accumulation layer at the InAs(111)A/B surfaces.

In the second part, high-resolution synchrotron based angle-resolved PES (ARPES) data from the cuprate high-temperature superconductor La(2-x)Sr(x)CuO(4) (LSCO) is presented. This extensive study, reveals detailed information about how the Fermi surface and electronic excitations evolve with doping in the superconducting state. The results comprise support for a connection between high- and low-energy electronic responses, the characteristics of the superconducting gap, and indication of a quantum phase transition between two different superconducting phases.

In the third group of experiments we move away from the two-dimensional systems and concentrate on fully three-dimensional compounds. By the use of soft x-ray ARPES it is possible to extract the three-dimensional electronic structure in a straightforward manner with increased k(perpendicular)-resolution. As a result the first high-quality ARPES data from Cu2O is presented, as well as a novel method for extracting the (real space) electron density by ARPES. These experiments clearly display the advantages of using soft x-ray ARPES. If the material and type of experiment is chosen wisely, the benefit of the increased k||-window and the free electron final state, surpass the drawbacks of decreased count-rate and inferior energy resolution. Finally we return to the high-temperature superconductors (NCCO & Nd-LSCO) and make use of the increased bulk-sensitivity. From an evident change in the shape of the Fermi surface when moving from low to high photon energies, the durface to bulk difference in electronic structure is highlighted.

Place, publisher, year, edition, pages
Stockholm: KTH , 2007. , xvi, 54 p.
Series
Trita-ICT/MAP, 2007:12
Keyword [en]
angle-resolved photoelectron spectroscopy, electronic structure, electron dynamics, semiconductor surfaces, oxides, high-temperature superconductors
National Category
Other Engineering and Technologies not elsewhere specified
Identifiers
URN: urn:nbn:se:kth:diva-4659ISBN: 978-91-7178-822-1 (print)OAI: oai:DiVA.org:kth-4659DiVA: diva2:13289
Public defence
2007-12-13, N1, Isafjordsgatan 28 A/D, Kista, 10:15
Opponent
Supervisors
Note
QC 20100810Available from: 2007-12-12 Created: 2007-12-12 Last updated: 2010-08-10Bibliographically approved
List of papers
1. Electronic structure and electron dynamics of delocalized adatom states at the Ge(111)c(2 x 8) surface
Open this publication in new window or tab >>Electronic structure and electron dynamics of delocalized adatom states at the Ge(111)c(2 x 8) surface
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(English)In: Physical Review B, ISSN 1098-0121Article in journal (Refereed) In press
National Category
Other Engineering and Technologies not elsewhere specified
Identifiers
urn:nbn:se:kth:diva-8055 (URN)
Note
QC 20100810Available from: 2007-12-12 Created: 2007-12-12 Last updated: 2010-08-10Bibliographically approved
2. Ultrafast electron dynamics and recombination at the Ge(111): Sn(root 3 X root 3)R30 degrees surface
Open this publication in new window or tab >>Ultrafast electron dynamics and recombination at the Ge(111): Sn(root 3 X root 3)R30 degrees surface
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2008 (English)In: Surface Science Letters, ISSN 0039-6028, Vol. 602, no 5, L33-L37 p.Article in journal (Refereed) Published
Abstract [en]

We present the first study revealing the electronic structure and electron dynamics of the excited adatom state at the Ge(111): Sn(root 3 x root 3)R30 degrees surface. By the use of time- and angle-resolved photoemission spectroscopy, the normally unoccupied electronic structure of the partly empty Sn adatom can be probed. From the angle-resolved data we conclude that the adatom electrons at the Ge:Sn surface are more delocalized than at the clean Ge(111)c(2 x 8) surface. A unique pump-and-probe technique, based on a pulsed femtosecond laser-system, has also allowed us to study the recombination process of the excited state. We connect the recombination process of the excited electrons to the coherent fluctuations of the Sn adatoms. As a result we present an estimate for the time between each collective and coherent adatom flip Delta t = 9 ps, i.e. an adatom switching frequency nu(SW) approximate to 0.1 THz. We find that our results, contrary to scanning tunneling microscopy measurements [F. Ronci, S. Colonna, S.D. Thorpe, A. Cricenti, G. Le Lay, Phys. Rev. Lett. 95 (2005) 156101], agree very well with values extracted from molecular dynamics simulations found in the literature [J. Avila, A. Mascaraque, E.G. Michel, M.C. Asensio, G. Le Lay, J. Ortega, R. Perez, F. Flores, Phys. Rev. Lett. 82 (1999) 442; D. Farias, W. Kaminski, J. Lobo, J. Ortega, E. Hulpke, R. Perez, F. Flores, E.G. Michel, Phys. Rev. Lett. 91 (2003) 16103].

Keyword
laser spectroscopy; time-resolved spectroscopy; angle-resolved photoemission; excited state; CHARGE-DENSITY-WAVE; PHASE-TRANSITION; SN/GE(111); FLUCTUATIONS; SN/GE(III)
National Category
Other Engineering and Technologies not elsewhere specified
Identifiers
urn:nbn:se:kth:diva-8056 (URN)10.1016/j.susc.2008.01.015 (DOI)000254801800002 ()2-s2.0-39749184684 (Scopus ID)
Note
QC 20100810Available from: 2007-12-12 Created: 2007-12-12 Last updated: 2012-03-20Bibliographically approved
3. Coherent d-wave superconducting gap in underdoped La2-xSrxCuO4 by angle-resolved photoemission spectroscopy
Open this publication in new window or tab >>Coherent d-wave superconducting gap in underdoped La2-xSrxCuO4 by angle-resolved photoemission spectroscopy
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2008 (English)In: Physical Review Letters, ISSN 0031-9007, Vol. 101, no 4, 047002- p.Article in journal (Refereed) Published
Abstract [en]

We present angle-resolved photoemission spectroscopy data on moderately underdoped La1.855Sr0.145CuO4 at temperatures below and above the superconducting transition temperature. Unlike previous studies of this material, we observe sharp spectral peaks along the entire underlying Fermi surface in the superconducting state. These peaks trace out an energy gap that follows a simple d-wave form, with a maximum superconducting gap of 14 meV. Our results are consistent with a single gap picture for the cuprates. Furthermore our data on the even more underdoped sample La1.895Sr0.105CuO4 also show sharp spectral peaks, even at the antinode, with a maximum superconducting gap of 26 meV.

Keyword
Copper compounds; Electric conductivity; Emission spectroscopy; Luminescence of organic solids; Photoelectricity; Photoemission; Superconducting transition temperature; Superconductivity;American Physical Society (APS); Angle-resolved photoemission spectroscopy (ARPES); Cuprates; La2 xSrxCuO4 (LSCO); Spectral peaks; Superconducting gaps; Superconducting states; Superconducting transitions; Wave forms; Gallium alloys
National Category
Other Engineering and Technologies not elsewhere specified
Identifiers
urn:nbn:se:kth:diva-8057 (URN)10.1103/PhysRevLett.101.047002 (DOI)000258427100049 ()2-s2.0-48049100977 (Scopus ID)
Note
QC 20100810. Uppdaterad från In press till Published, titel ändrad, tidigare titel: "The coherent d-wave superconducting gap in underdoped La(1.855)Sr(0.145)CuO4) as studied by angle-resolved photoemission" 20100810.Available from: 2007-12-12 Created: 2007-12-12 Last updated: 2010-08-12Bibliographically approved
4. Angle Resolved Photoemission from Nd(1.85)Ce(0.15)CuO(4) using High Energy Photons: A Fermi Surface Investigation
Open this publication in new window or tab >>Angle Resolved Photoemission from Nd(1.85)Ce(0.15)CuO(4) using High Energy Photons: A Fermi Surface Investigation
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2004 (English)In: Physical Review Letters, ISSN 0031-9007, Vol. 93, no 13, 136402-1-136402-4 p.Article in journal (Refereed) Published
Abstract [en]

We have performed an angle resolved photoemission study on a single crystal of the optimally electron doped (n-type) cuprate superconductor Nd2-xCexCuO4 (x=0.15) at a photon energy of 400 eV. The Fermi surface is mapped out and is, in agreement with earlier measurements, of hole-type with the expected Luttinger volume. However, comparing with previous low energy measurements, we observe a different Fermi surface shape and a different distribution of spectral intensity around the Fermi surface contour. The observed Fermi surface shape indicates a stronger electron correlation in the bulk as compared to the surface.

Keyword
Antiferromagnetism; Doping (additives); Electric power measurement; Electron energy analyzers; Electronic structure; Electrons; Fermi surface; Neodymium compounds; Oxide superconductors; Photons; Single crystals; Synchrotron radiation
National Category
Condensed Matter Physics Other Engineering and Technologies not elsewhere specified
Identifiers
urn:nbn:se:kth:diva-8058 (URN)10.1103/PhysRevLett.93.136402 (DOI)000224131400061 ()2-s2.0-19644397887 (Scopus ID)
Note
QC 20100702 QC 20110916Available from: 2007-12-12 Created: 2007-12-12 Last updated: 2011-09-16Bibliographically approved
5. The electronic structure of La(1.48)Nd(0.4)Sr(0.12)CuO(4) probed by high- and low-energy angle-resolved photoelectron spectroscopy: Evolution with probing depth
Open this publication in new window or tab >>The electronic structure of La(1.48)Nd(0.4)Sr(0.12)CuO(4) probed by high- and low-energy angle-resolved photoelectron spectroscopy: Evolution with probing depth
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2009 (English)In: Physical Review B Condensed Matter, ISSN 0163-1829, E-ISSN 1095-3795, Vol. 80, no 9, 094503-1-094503-6 p.Article in journal (Refereed) Published
Abstract [en]

We present angle-resolved photoelectron spectroscopy data probing the electronic structure of the Nd-substituted high-T-c cuprate La1.48Nd0.4Sr0.12CuO4. Data have been acquired at low and high photon energies, h nu=55 and 500 eV, respectively. The two extracted Fermi surfaces show significant differences. The differences can be attributed to either the change in probing depth suggesting dissimilarity of the intrinsic electronic structure between surface and bulk regions, or a considerable c-axis dispersion signaling a strong interlayer coupling. At both photon energies, considerable spectral weight is observed at all points along the Fermi surface and the intensity distribution as well as Fermi-surface shape observed at low as well as high photon energy is markedly different from what has been previously reported for La1.28Nd0.6Sr0.12CuO4 by Zhou [Science 286, 268 (1999)]. Document Type: Article

Keyword
band structure; Fermi surface; high-temperature superconductors; lanthanum compounds; neodymium; photoelectron spectra; strontium compounds
National Category
Other Engineering and Technologies not elsewhere specified
Identifiers
urn:nbn:se:kth:diva-8059 (URN)10.1103/PhysRevB.80.094503 (DOI)000270383000073 ()2-s2.0-70349974665 (Scopus ID)
Note
QC 20100702Available from: 2007-12-12 Created: 2007-12-12 Last updated: 2010-07-02Bibliographically approved
6. Anisotropy of electron structure at InAs(111) surfaces by laser pump-and-probe photoemission spectroscopy
Open this publication in new window or tab >>Anisotropy of electron structure at InAs(111) surfaces by laser pump-and-probe photoemission spectroscopy
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2005 (English)In: Surface Science, ISSN 0039-6028, E-ISSN 1879-2758, Vol. 574, no 1, 89-94 p.Article in journal (Refereed) Published
Abstract [en]

The electronic structure and the electron dynamics of the clean InAs(111)A 2 x 2 and the InAs(111)B 1 x 1 surfaces have been studied by laser pump-and-probe photoemission spectroscopy. Normally unpopulated electron states above the valence band maximum (VBM) are filled on the InAs(111)A surface due to the conduction band pinning above the Fermi level (E-F). Accompanied by the downward band banding alignment, a charge accumulation layer is confined to the surface region creating a two dimensional electron gas (2DEG). The decay of the photoexcited carriers above the conduction band minimum (CBM) is originated by bulk states affected by the presence of the surface. No occupied states were found on the InAs(111)B 1 x 1 surface. This fact is suggested to be due to the surface stabilisation by the charge removal from the surface into the bulk. The weak photoemission intensity above the VBM on the (111)B surface is attributed to electron states trapped by surface defects. The fast decay of the photoexcited electron states on the (111)A and the (111)B surfaces was found to be tau(111A) less than or equal to 5 ps and tau(111B) less than or equal to 4ps, respectively. We suggest the diffusion of the hot electrons into the bulk is the decay mechanism. (

Keyword
Angle resolved photoemission; Indium arsenide; Laser methods; Surface electronic phenomena (work function, surface potential, surface states, etc.); Anisotropy; Electron energy levels; Electron gas; Fermi level; Heterojunctions; Molecular beam epitaxy; Photoemission; Indium compounds
National Category
Other Engineering and Technologies not elsewhere specified
Identifiers
urn:nbn:se:kth:diva-8060 (URN)10.1016/j.susc.2004.10.018 (DOI)000226214400010 ()2-s2.0-10844273387 (Scopus ID)
Note
QC 20100810Available from: 2007-12-12 Created: 2007-12-12 Last updated: 2010-10-15Bibliographically approved
7. Electronic structure and electron dynamics at the GaSb(001) surface studied by femtosecond pump-and-probe pulsed laser photoemission spectroscopy
Open this publication in new window or tab >>Electronic structure and electron dynamics at the GaSb(001) surface studied by femtosecond pump-and-probe pulsed laser photoemission spectroscopy
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2006 (English)In: Applied Surface Science, ISSN 0169-4332, E-ISSN 1873-5584, Vol. 252, no 15, 5308-5311 p.Article in journal (Refereed) Published
Abstract [en]

Transiently excited electron states at the GaSb(001) surface have been studied by means of time- and angle-resolved photoemission spectroscopy based on a femtosecond laser system. A normally unpopulated surface electron state has been found at similar to 250 meV above the valence band maximum with a strong confinement at the center of the surface Brillouin zone. The lifetime of transiently excited carriers at the intergap surface states has been found to be similar to 11 ps, associated with rapid carrier diffusion.

Keyword
Angle-resolved photoemission; Gallium antimonide; Laser methods; Photoelectron emission; Surface states; Diffusion; Electrodynamics; Electronic structure; Laser theory; Photoemission; Spectroscopic analysis; Semiconducting gallium compounds
National Category
Other Engineering and Technologies not elsewhere specified
Identifiers
urn:nbn:se:kth:diva-8061 (URN)10.1016/j.apsusc.2005.12.138 (DOI)000238623300017 ()2-s2.0-33746802374 (Scopus ID)
Note

QC 20100810. Titel ändrad, tidigare titel: "Electron structure and electron dynamics at the GaSb(001) surface studied by femtosecond pump-and-probe pulsed laser surface studied by femtosecond pump-and-probe pulsed laser" 20100810. Konferens: 8th International Conference on Atomically Controlled Surfaces, Interfaces, and Nanostructures/13th International Congress on Thin Films, Stockholm, 2005.

Available from: 2007-12-12 Created: 2007-12-12 Last updated: 2016-12-21Bibliographically approved
8. Revealing the charge density in solids
Open this publication in new window or tab >>Revealing the charge density in solids
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(English)Manuscript (Other academic)
National Category
Other Engineering and Technologies not elsewhere specified
Identifiers
urn:nbn:se:kth:diva-8062 (URN)
Note
QC 20100702Available from: 2007-12-12 Created: 2007-12-12 Last updated: 2010-07-02Bibliographically approved
9. Probing the valence band structure of Cu2O using high-energy angle-resolved photoelectron spectroscopy
Open this publication in new window or tab >>Probing the valence band structure of Cu2O using high-energy angle-resolved photoelectron spectroscopy
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2007 (English)In: Physical Review B Condensed Matter, ISSN 0163-1829, E-ISSN 1095-3795, Vol. 76, no 11, 115127-1-115127-7 p.Article in journal (Refereed) Published
Abstract [en]

We present angle-resolved photoemission data along the M-Gamma-M direction from a Cu2O(111) single crystal, collected at high photon energies (h nu=619 and 891 eV) and T=100 K. Because of the high photon energies and effective background subtraction, our data give a clear picture of the bulk band structure. The results confirm the existence of a hybridized Cu 3d-Cu 4s state located between the two main Cu 3d and O 2p band regions. Several theoretical studies have predicted the existence of this band, but until now it has not been detected in any photoemission measurements. The experimentally derived band structure is compared to local density approximation calculations with and without the Hubbard potential U. The clear band dispersion in our experimental data has enabled us to extract a refined Hubbard U value, which makes it possible to achieve a better agreement between theoretically calculated bands and experimental data.

Keyword
CLOSED-SHELL INTERACTIONS; ELECTRONIC-STRUCTURE; SYNCHROTRON-RADIATION; POLAR COVALENCES; CUPROUS-OXIDE; DIRECT IMAGES; PHOTOEMISSION; CUPRITE; CUO; SPECTRA
National Category
Other Engineering and Technologies not elsewhere specified
Identifiers
urn:nbn:se:kth:diva-8063 (URN)10.1103/PhysRevB.76.115127 (DOI)000249786400046 ()2-s2.0-34848905947 (Scopus ID)
Note
QC 20100702Available from: 2007-12-12 Created: 2007-12-12 Last updated: 2012-03-20Bibliographically approved
10. On-board sample cleaver
Open this publication in new window or tab >>On-board sample cleaver
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2007 (English)In: Review of Scientific Instruments, ISSN 0034-6748, E-ISSN 1089-7623, Vol. 78, no 7, 076103- p.Article in journal (Refereed) Published
Abstract [en]

An on-board sample cleaver has been developed in order to cleave small and hard-to-cleave samples. To acquire good cleaves from rigid samples the alignment of the cleaving blade with respect to the internal crystallographic planes is crucial. To have the opportunity to mount the sample and align it to the blade ex situ has many advantages. The design presented has allowed us to cleave very tiny and rigid samples, e.g., the high-temperature superconductor La(2-x)SrxCuO4. Further, in this design the sample and the cleaver will have the same temperature, allowing us to cleave and keep the sample at low temperature. This is a big advantage over prior cleaver systems. As a result, better surfaces and alignments can be realized, which considerably simplifies and improves the experiments.

Keyword
High temperature superconductors; Low temperature effects; Machine design; Sampling; Cleaving blades; Rigid samples; Sample design; Crystallography; article; electronics; equipment; equipment design; instrumentation; laboratory diagnosis; materials testing; methodology; microtomy; reproducibility; sensitivity and specificity; system analysis; Equipment Design; Equipment Failure Analysis; Materials Testing; Microtomy; Miniaturization; Reproducibility of Results; Sensitivity and Specificity; Specimen Handling; Systems Integration
National Category
Other Engineering and Technologies not elsewhere specified
Identifiers
urn:nbn:se:kth:diva-8064 (URN)10.1063/1.2756754 (DOI)000248486300072 ()17672802 (PubMedID)2-s2.0-34547574333 (Scopus ID)
Note
QC 20100810Available from: 2007-12-12 Created: 2007-12-12 Last updated: 2012-03-20Bibliographically approved
11. When low- and high-energy electronic responses meet in cuprate superconductors
Open this publication in new window or tab >>When low- and high-energy electronic responses meet in cuprate superconductors
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2007 (English)In: Physical Review B. Condensed Matter and Materials Physics, ISSN 1098-0121, E-ISSN 1550-235X, Vol. 75, no 22, 224508- p.Article in journal (Refereed) Published
Abstract [en]

The existence of coherent quasiparticles near the Fermi energy in the low-temperature state of high-temperature superconductors has been well established by angle-resolved photoemission spectroscopy (ARPES). We present a study of La1.83Sr0.17CuO4 in the superconducting state and report an abrupt change in the quasiparticle spectral function, as we follow the dispersion of the ARPES signal from the Fermi energy to 0.6 eV. The interruption in the quasiparticle dispersion separates coherent quasiparticle peaks at low energies from broad incoherent excitations at high energies. We find that the boundary between these low-energy and high-energy features exhibits a cosine-shaped momentum dependence, reminiscent of the superconducting d-wave gap. Further intriguing similarities between characteristics of the incoherent excitations and quasiparticle properties suggest a close relation between the electronic response at high and low energies in cuprate superconductors.

Keyword
HIGH-TEMPERATURE SUPERCONDUCTORS; T-C SUPERCONDUCTORS; EXCITATIONS; OXIDES; MODE
National Category
Other Engineering and Technologies not elsewhere specified
Identifiers
urn:nbn:se:kth:diva-8065 (URN)10.1103/PhysRevB.75.224508 (DOI)000247624800090 ()2-s2.0-34347358510 (Scopus ID)
Note
QC 20100810Available from: 2007-12-12 Created: 2007-12-12 Last updated: 2010-08-10Bibliographically approved
12. Anisotropic quasiparticle scattering rates in slightly underdoped to optimally doped high-temperature La2-xSrxCuO4 superconductors
Open this publication in new window or tab >>Anisotropic quasiparticle scattering rates in slightly underdoped to optimally doped high-temperature La2-xSrxCuO4 superconductors
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2008 (English)In: Physical Review B. Condensed Matter and Materials Physics, ISSN 1098-0121, E-ISSN 1550-235X, Vol. 78, no 20, 205103- p.Article in journal (Refereed) Published
Abstract [en]

An angle-resolved photoemission study of the scattering rate in the superconducting phase of the high-temperature superconductor La2-xSrxCuO4 with x=0.145 and x=0.17, as a function of binding energy and momentum, is presented. We observe that the scattering rate scales linearly with binding energy up to the high-energy scale E-1 similar to 0.4 eV. The scattering rate is found to be strongly anisotropic, with a minimum along the (0,0)-(pi,pi) direction. A possible connection to a quantum-critical point is discussed.

Keyword
NORMAL-STATE; BI2SR2CACU2O8+DELTA
National Category
Other Engineering and Technologies not elsewhere specified
Identifiers
urn:nbn:se:kth:diva-8066 (URN)10.1103/PhysRevB.78.205103 (DOI)000261215400016 ()2-s2.0-56349092270 (Scopus ID)
Note
QC 20100810. Uppdaterad från In press till Published. Tidigare titel: Anisotropic scattering in slightly underdoped to optimally doped La(2-x)Sr(x)CuO(4). 20100810.Available from: 2007-12-12 Created: 2007-12-12 Last updated: 2010-08-12Bibliographically approved
13. Experimental evidence of a quantum phase transition in La(2-x)Sr(x)CuO4()
Open this publication in new window or tab >>Experimental evidence of a quantum phase transition in La(2-x)Sr(x)CuO4()
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(English)Manuscript (Other academic)
National Category
Other Engineering and Technologies not elsewhere specified
Identifiers
urn:nbn:se:kth:diva-8067 (URN)
Note
QC 20100702Available from: 2007-12-12 Created: 2007-12-12 Last updated: 2010-08-10Bibliographically approved

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