| 1. |
- Sanchez-Gonzalez, A., et al.
(författare)
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Accurate prediction of X-ray pulse properties from a free-electron laser using machine learning
- 2017
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 8
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Tidskriftsartikel (refereegranskat)abstract
- Free-electron lasers providing ultra-short high-brightness pulses of X-ray radiation have great potential for a wide impact on science, and are a critical element for unravelling the structural dynamics of matter. To fully harness this potential, we must accurately know the X-ray properties: intensity, spectrum and temporal profile. Owing to the inherent fluctuations in free-electron lasers, this mandates a full characterization of the properties for each and every pulse. While diagnostics of these properties exist, they are often invasive and many cannot operate at a high-repetition rate. Here, we present a technique for circumventing this limitation. Employing a machine learning strategy, we can accurately predict X-ray properties for every shot using only parameters that are easily recorded at high-repetition rate, by training a model on a small set of fully diagnosed pulses. This opens the door to fully realizing the promise of next-generation high-repetition rate X-ray lasers.
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| 2. |
- Rohringer, N., et al.
(författare)
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Stimulated X-Ray Raman Scattering with Free-Electron Laser Sources
- 2016
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Ingår i: X-Ray Lasers 2014. - Cham : Springer. - 0930-8989. - 9783319195216 - 9783319195209 ; , s. 201-207
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Bokkapitel (refereegranskat)abstract
- Stimulated electronic x-ray Raman scattering is the building block for several proposed x-ray pump probe techniques, that would allow the study of electron dynamics at unprecedented timescales.We present high spectral resolution data on stimulated electronic x-ray Raman scattering in a gas sample of neon using a self-amplified spontaneous emission x-ray free-electron laser. Despite the limited spectral coherence and broad bandwidth of these sources, high-resolution spectra can be obtained by statistical methods, opening the path to coherent stimulated x-ray Raman spectroscopy. An extension of these ideas to molecules and the results of a recent experiment in CO are discussed.
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| 3. |
- Sanchez-Gonzalez, A., et al.
(författare)
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Auger electron and photoabsorption spectra of glycine in the vicinity of the oxygen K-edge measured with an X-FEL
- 2015
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Ingår i: Journal of Physics B-Atomic Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 48:23
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Tidskriftsartikel (refereegranskat)abstract
- We report the first measurement of the near oxygen K-edge auger spectrum of the glycine molecule. Our work employed an x-ray free electron laser as the photon source operated with input photon energies tunable between 527 and 547 eV. Complete electron spectra were recorded at each photon energy in the tuning range, revealing resonant and non-resonant auger structures. Finally ab initio theoretical predictions are compared with the measured above the edge auger spectrum and an assignment of auger decay channels is performed.
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| 4. |
- Zitnik, M, et al.
(författare)
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High resolution multiphoton spectroscopy by a tunable free-electron-laser light.
- 2014
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Ingår i: Physical Review Letters. - 1079-7114 .- 0031-9007. ; 113:19
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Tidskriftsartikel (refereegranskat)abstract
- Seeded free electron lasers theoretically have the intensity, tunability, and resolution required for multiphoton spectroscopy of atomic and molecular species. Using the seeded free electron laser FERMI and a novel detection scheme, we have revealed the two-photon excitation spectra of dipole-forbidden doubly excited states in helium. The spectral profiles of the lowest (-1,0)^{+1} ^{1}S^{e} and (0,1)^{0} ^{1}D^{e} resonances display energy shifts in the meV range that depend on the pulse intensity. The results are explained by an effective two-level model based on calculated Rabi frequencies and decay rates.
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| 5. |
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| 6. |
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| 7. |
- Agui, A., et al.
(författare)
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Direct observation of interface effects of thin AlAs(100) layers buried in GaAs
- 2000
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Ingår i: Applied Surface Science. - : Elsevier. - 0169-4332 .- 1873-5584. ; 166:1-4, s. 309-312
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Tidskriftsartikel (refereegranskat)abstract
- A study of the electronic structure of ultrathin AlAs layers buried in GaAs(100) and their interfaces is presented. Al L2,3 soft-X-ray-emission (SXE) spectra from the AlAs layers were measured. The spectra show distinct thickness-dependent features, which are reproduced using ab initio calculations.
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| 8. |
- Butorin, S. M., et al.
(författare)
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Probing the Mn3+ sublattice in La0.5Ca0.5MnO3 by resonant inelastic soft X-ray scattering at the MnL2,3 edge
- 2002
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Ingår i: Surface review and letters. - : World Scientific. - 0218-625X .- 1793-6667. ; 9:2, s. 989-992
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Tidskriftsartikel (refereegranskat)abstract
- Resonant soft X-ray scattering spectra of a La0.5Ca0.5MnO3 thin film were measured at varying energies of the incident photon beam across Mn 2p thresholds. The data are analyzed within the framework of the Anderson impurity model and full multiplet theory. The scattering profiles of the film are reasonably well reproduced by model calculations for the Mn3+ system, in contrast to the absorption spectrum at the Mn L2,L3 edge for which the contribution of the Mn4+ sublattice is required to be taken into account. The obtained agreement between calculations and experiment indicates that in this case resonant inelastic scattering mainly probes the local electronic structure at the Mn3+ sites in the La0.5Ca0.5MnO3 film. In turn, Mn4+ sites mainly contribute to ordinary L-alpha,L-beta X-ray emission due to relaxations in the intermediate state of the spectroscopic process. Such a situation can occur when the system favors a phase separation rather than checkerboard charge ordering of Mn3+ and Mn4+ sites.
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| 9. |
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| 10. |
- Couto, Rafael C., et al.
(författare)
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Anomalously strong two-electron one-photon X-ray decay transitions in CO caused by avoided crossing
- 2016
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Ingår i: Scientific Reports. - : Nature Publishing Group. - 2045-2322. ; 6
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Tidskriftsartikel (refereegranskat)abstract
- The unique opportunity to study and control electron-nuclear quantum dynamics in coupled potentials offered by the resonant inelastic X-ray scattering (RIXS) technique is utilized to unravel an anomalously strong two-electron one-photon transition from core-excited to Rydberg final states in the CO molecule. High-resolution RIXS measurements of CO in the energy region of 12-14 eV are presented and analyzed by means of quantum simulations using the wave packet propagation formalism and ab initio calculations of potential energy curves and transition dipole moments. The very good overall agreement between the experimental results and the theoretical predictions allows an in-depth interpretation of the salient spectral features in terms of Coulomb mixing of "dark" with "bright" final states leading to an effective two-electron one-photon transition. The present work illustrates that the improved spectral resolution of RIXS spectra achievable today may call for more advanced theories than what has been used in the past.
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| 11. |
- Couto, Rafael C., et al.
(författare)
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Coupled electron-nuclear dynamics in resonant 1σ→2π x-ray Raman scattering of CO molecules
- 2016
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Ingår i: Physical Review A (Atomic, Molecular and Optical Physics). - 1050-2947. ; 93:3
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Tidskriftsartikel (refereegranskat)abstract
- We present a detailed experimental-theoretical analysis of O K-edge resonant 1σ-2π inelastic x-ray scattering (RIXS) from carbon monoxide with unprecedented energy resolution. We employ high-level ab initio calculations to compute the potential energy curves of the states involved in the RIXS process and simulate the measured RIXS spectra using the wave-packet-propagation formalism, including Coulomb coupling in the final-state manifold. The theoretical analysis allows us to explain all the key features of the experimental spectra, including some that were not seen before. First, we clearly show the interference effect between different RIXS channels corresponding to the transition via orthogonal Πx1 and Πy1 core-excited states of CO. Second, the RIXS region of 13 eV energy loss presents a triple structure, revealed only by the high-resolution measurement. In previous studies, this region was attributed solely to a valence state. Here we show a strong Coulomb mixing of the Rydberg and valence final states, which opens the forbidden RIXS channels to the "dark" final Rydberg states and drastically changes the RIXS profile. Third, using a combination of high-resolution experiment and high-level theory, we improve the |4σ-12π1) final-state potential-energy curve by fitting its bottom part with the experiment. Also, the coupling constants between Rydberg and valence states were refined via comparison with the experiment. Our results illustrate the large potential of the RIXS technique for advanced studies of highly excited states of neutral molecules.
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| 12. |
- Eichmann, U., et al.
(författare)
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Photon-recoil imaging : Expanding the view of nonlinear x-ray physics
- 2020
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Ingår i: Science. - : AMER ASSOC ADVANCEMENT SCIENCE. - 0036-8075 .- 1095-9203. ; 369:6511, s. 1630-1633
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Tidskriftsartikel (refereegranskat)abstract
- Addressing the ultrafast coherent evolution of electronic wave functions has long been a goal of nonlinear x-ray physics. A first step toward this goal is the investigation of stimulated x-ray Raman scattering (SXRS) using intense pulses from an x-ray free-electron laser. Earlier SXRS experiments relied on signal amplification during pulse propagation through dense resonant media. By contrast, our method reveals the fundamental process in which photons from the primary radiation source directly interact with a single atom. We introduce an experimental protocol in which scattered neutral atoms rather than scattered photons are detected. We present SXRS measurements at the neon K edge and a quantitative theoretical analysis. The method should become a powerful tool in the exploration of nonlinear x-ray physics.
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| 13. |
- Gunnelin, K, et al.
(författare)
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Bond-length-dependent core hole localization observed in simple hydrocarbons
- 1999
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Ingår i: Physical Review Letters. - 0031-9007. ; 83:7, s. 1315-1318
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Tidskriftsartikel (refereegranskat)abstract
- Soft x-ray-emission spectroscopy is applied to measure the amount of dynamic symmetry breaking in core-excited acetylene, ethylene, and ethane. Large variations are observed between the molecules and are rationalized in terms of the different C-C bond lengths: Shorter bond lengths give smaller symmetry breaking. The results also indicate that asymmetric modes are important for all the systems studied, in contradiction to previous assumptions in literature.
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| 14. |
- Guo, J. H., et al.
(författare)
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Characterization of undulator radiation at MAXII using a soft X-ray fluorescence spectrometer
- 1999
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Ingår i: Nuclear Instruments & Methods in Physics Research. Section A: Accelerators, Spectrometers, Detectors, and Associated Equipment. - 0168-9002. ; 431:1, s. 285-293
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Tidskriftsartikel (refereegranskat)abstract
- A grazing-incidence grating spectrometer has been used for the investigation of the undulator radiation from beamline 411 at MAX-lab. The direct detection of undulator light is expected to obtain the information of the quality of the undulator. Regular undulator radiation and some higher harmonics were observed. The effects of electronic beam coupling and Landau cavities have been studied. The experiment presents an easy and quick method to characterize the undulator radiation before the permanent monochromator is installed.
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| 15. |
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| 16. |
- Guo, J.-H., et al.
(författare)
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How the phenyle rings (benzene) act as building blocks in pi conjugated polymers
- 1998
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Ingår i: Advanced Light Source. - Berkeley : Ernest Orlando Lawrence Berkeley National Laboratory, University of California Berkeley, California, USA. ; , s. 129-132
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Bokkapitel (övrigt vetenskapligt/konstnärligt)abstract
- Organic conjugated polymers have the electronic structure of semiconductors and can be doped to become good conductors (1). Conjugated polymers are now used as active materials in a wide variety of prototype applications such as light emitting diodes [2] and organic transistors [3,4]. Most of the interesting chemistry and physics of conjugated polymers is associated with the details of the electronic structure at the valence and conduction band edges and, in this connection, various electron spectroscopies can be used as tools for diagnosis of the relevant electronic and geometric properties....
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| 17. |
- Guo, J.-H., et al.
(författare)
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Resonant and nonresonant x-ray scattering spectra of some poly(phenylenevinylene)s
- 1998
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 108:14, s. 5990-5996
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Tidskriftsartikel (refereegranskat)abstract
- 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, indicating a local character of the x-ray emission in which the phenyl ring acts as a building block. Theoretical simulations of x-ray energies and intensities taking the repeat unit as a model molecule of the polymer agree with the experimental spectra fairly well. The edges of the occupied bands have been identified in the nonresonant spectra of each polymer. By subtracting the emission energy of the highest occupied molecular orbital in the nonresonant spectrum from the core excitation energy in the resonant spectrum an alternative way to determine the optical band gap is obtained. As for free benzene the outer π band in the polymer spectra show a depletion of the emission going from the nonresonant to the resonant x-ray emission spectra. It is demonstrated that this transition, which is strictly symmetry forbidden for free benzene, becomes effectively forbidden in the polymer case as a result of strong interference effects, and it is argued that this is the general case for resonant x-ray emission of conjugated polymers as far as the frozen orbital approximation holds.
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| 18. |
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| 19. |
- Kashtanov, Stepan, et al.
(författare)
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Local structures of liquid water studied by x-ray emission spectroscopy
- 2004
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Ingår i: Physical Review B. Condensed Matter and Materials Physics. - 1098-0121 .- 1550-235X. ; 69:2
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Tidskriftsartikel (refereegranskat)abstract
- The O Kalpha x-ray emission spectra of water clusters with different sizes and conformations embedded in a continuum medium are simulated. The calculations have successfully explained the experimental spectra of water in both gas and liquid phases. It is shown that the x-ray emission spectra are very sensitive to the local hydrogen bonding structures. Strong electron sharing between different water molecules is observed and its possible connection to the covalency of hydrogen bonding is discussed. The experimentally observed strong excitation energy dependence of the spectra has been interpreted in terms of the polarization and angular dependence for the gas phase, and in terms of variations of local hydrogen bonding structures for the liquid phase.
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| 20. |
- Kjellsson, Ludvig, et al.
(författare)
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Resonant inelastic x-ray scattering at the N2 π*-resonance: Lifetime-vibrational interference, radiative electron rearrangement, and wave-function imaging
- 2021
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Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - : American Physical Society. - 1050-2947 .- 1094-1622. ; 103
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Tidskriftsartikel (refereegranskat)abstract
- Resonant inelastic x-ray scattering spectra excited at the pi*-resonance of the nitrogen molecule are presented. Well-resolved vibrational excitations in the electronic ground state, and in the 3 sigma g(-1 )1 pi(1)(g) a(1) Pi(g) state are observed. The spectra are analyzed within the Kramers-Heisenberg formalism, and the importance of lifetime-vibrational interference effects is highlighted. In addition, strongly dissociative multiply excited final states populated in radiative electron rearrangement are found in the valence ionization continua. The vibrational wave functions of the core-excited state are imaged on the strongly dissociative final state potentials.
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| 21. |
- Käämbre, T, et al.
(författare)
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Study of oxygen-C compound formation by NEXAFS and RIXS
- 2001
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Ingår i: The European Physical Journal D. ; 16:1-3, s. 357-360
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Tidskriftsartikel (refereegranskat)abstract
- The interaction of oxygen with C60 molecules was studied on a C60 film which had been exposed simultaneously to oxygen and UV-light for 190 hours, producing an approximately C60O1 stoichiometry in the bulk of the sample. C K-edge and O K-edge NEXAFS (using total fluorescence yield detection) and resonant X-ray inelastic scattering (RIXS) spectra from the sample film were measured and the C K-edge data were compared to the spectra from pristine C60 as reference. The C K-edge absorption and emission spectral profiles of the oxygen-doped sample are similar to those of the C60 reference, suggesting that cage breaking of C60 under these conditions, if any, is negligible. However, the redistribution of intensities in the spectra indicates changes in the occupancies of different molecular orbitals, possibly due to changes in electron density upon reaction. Similarities of the O K-edge soft X-ray emission (SXES) spectra to several small oxygen-containing molecules is being discussed in terms of bonding models.
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| 22. |
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| 23. |
- Magnuson, Martin, 1965-, et al.
(författare)
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Magnetic circular dichroism in X-ray fluorescence of Heuseler alloys at threshold excitation
- 2001
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Ingår i: Solid State Communications. - 0038-1098 .- 1879-2766. ; 117:2, s. 79-82
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Tidskriftsartikel (refereegranskat)abstract
- The results of fluorescence measurements of magnetic circular dichroism (MCD) in Mn L2,3 X-ray emission and absorption for Heusler alloys NiMnSb and Co2MnSb are presented. Very intense resonance Mn L3 emission is found at the Mn 2p3/2 threshold and attributed to a peculiarity of the threshold excitation in materials with a half-metallic character of the electronic structure. The excitation energy dependence of Mn L2,3 X-ray emission spectra (XES) was measured at beamline ID12B at the European Synchrotron Radiation Facility (ESRF, Grenoble) using 83% circularly polarized X-rays. A very large MCD effect found in XES is attributed to strong exchange splitting of spin-up and spin-down Mn 3d states. The anomalously high ratio of L2 emission intensity to L3 emission intensity is found.
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| 24. |
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| 25. |
- Mankefors, S., et al.
(författare)
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Theoretical investigation of the thickness dependence of soft-x-ray emission from thin AlAs(100) layers buried in GaAs
- 2000
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Ingår i: Physical Review B Condensed Matter. - : American Physical Society. - 0163-1829 .- 1095-3795. ; 61:8, s. 5540-5545
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Tidskriftsartikel (refereegranskat)abstract
- Ultrathin AlAs(100) layers of 1-, 2-, and 5-ML thickness buried in GaAs are investigated by ab initio calculations. Unique experimental soft-x-ray emission spectra are explained in terms of interface effects and changes with layer thickness are found in the density of states. Only the central layer in the 5-ML geometry is bulklike. A valence-band offset of 0.53 eV is also found for this structure, while no offset exists in the 1- and 2-ML cases. Very good agreement is achieved between theory and experiment.
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