Deconvolving Instrumental and Intrinsic Broadening in Excited State X-ray Spectroscopies

Intrinsic and experimental mechanisms frequently lead to broadening of spectral features in excited-state spectroscopies. For example, intrinsic broadening occurs in x-ray absorption spectroscopy (XAS) measurements of heavy elements where the core-hole lifetime is very short. On the other hand, nonresonant x-ray Raman scattering (XRS) and other energy loss measurements are more limited by instrumental resolution. Here, we demonstrate that the Richardson-Lucy (RL) iterative algorithm provides a robust method for deconvolving instrumental and intrinsic resolutions from typical XAS and XRS data. For the K-edge XAS of Ag, we find nearly complete removal of ~9.3 eV FWHM broadening from the combined effects of the short core-hole lifetime and instrumental resolution. We are also able to remove nearly all instrumental broadening in an XRS measurement of diamond, with the resulting improved spectrum comparing favorably with prior soft x-ray XAS measurements. We present a practical methodology for implementing the RL algorithm to these problems, emphasizing the importance of testing for stability of the deconvolution process against noise amplification, perturbations in the initial spectra, and uncertainties in the core-hole lifetime.Comment: 35 pages, 13 figure

Errors in Hellmann-Feynman Forces due to occupation number broadening, and how they can be corrected

In ab initio calculations of electronic structures, total energies, and forces, it is convenient and often even necessary to employ a broadening of the occupation numbers. If done carefully, this improves the accuracy of the calculated electron densities and total energies and stabilizes the convergence of the iterative approach towards self-consistency. However, such a boardening may lead to an error in the calculation of the forces. Accurate forces are needed for an efficient geometry optimization of polyatomic systems and for ab initio molecular dynamics (MD) calculations. The relevance of this error and possible ways to correct it will be discussed in this paper. The first approach is computationally very simple and in fact exact for small MD time steps. This is demonstrated for the example of the vibration of a carbon dimer and for the relaxation of the top layer of the (111)-surfaces of aluminium and platinum. The second, more general, scheme employs linear-response theory and is applied to the calculation of the surface relaxation of Al(111). We will show that the quadratic dependence of the forces on the broadening width enables an efficient extrapolation to the correct result. Finally the results of these correction methods will be compared to the forces obtained by using the smearing scheme, which has been proposed by Methfessel and Paxton.Comment: 6 pages, 5 figures, Scheduled tentatively for the issue of Phys. Rev. B 15 15 Dec 97 Other related publications can be found at http://www.rz-berlin.mpg.de/th/paper.htm

Direct and Simultaneous Observation of Ultrafast Electron and Hole Dynamics in Germanium

Understanding excited carrier dynamics in semiconductors is crucial for the development of photovoltaics and efficient photonic devices. However, overlapping spectral features in optical/NIR pump-probe spectroscopy often render assignments of separate electron and hole carrier dynamics ambiguous. Here, ultrafast electron and hole dynamics in germanium nanocrystalline thin films are directly and simultaneously observed by attosecond transient absorption spectroscopy (ATAS) in the extreme ultraviolet at the germanium M_{4,5}-edge (~30 eV). We decompose the ATAS spectra into contributions of electronic state blocking and photo-induced band shifts at a carrier density of 8*10^{20}cm^{-3}. Separate electron and hole relaxation times are observed as a function of hot carrier energies. A first order electron and hole decay of ~1 ps suggests a Shockley-Read-Hall recombination mechanism. The simultaneous observation of electrons and holes with ATAS paves the way for investigating few to sub-femtosecond dynamics of both holes and electrons in complex semiconductor materials and across junctions.Comment: Includes Supplementary Informatio

The dark matter halo shape of edge-on disk galaxies - II. Modelling the HI observations: methods

This is the second paper of a series in which we attempt to put constraints on the flattening of dark halos in disk galaxies. For this purpose, we observe the HI in edge-on galaxies, where it is in principle possible to measure the force field in the halo vertically and radially from gas layer flaring and rotation curve decomposition respectively. To calculate the force fields, we need to analyse the observed XV diagrams to accurately measure all three functions that describe the planar kinematics and distribution of a galaxy: the radial HI surface density, the rotation curve and the HI velocity dispersion. In this paper, we discuss the improvements and limitations of the methods previously used to measure these HI properties. We extend the constant velocity dispersion method to include determination of the HI velocity dispersion as a function of galactocentric radius and perform extensive tests on the quality of the fits. We will apply this 'radial decomposition XV modelling method' to our HI observations of 8 HI-rich, late-type, edge-on galaxies in the third paper of this series.Comment: Accepted for publication by Astronomy & Astrophysics. For a higher resolution version see http://www.astro.rug.nl/~vdkruit/jea3/homepage/12566.pd

Numerical Renormalization Group Analysis of Interacting Quantum Dots

Wilson's Numerical Renormalization Group (NRG) is so far the only nonperturbative technique that can reliably access low-energy properties of quantum impurity systems. We present a recent extension of the method, the DM-NRG, which yields highly accurate results for dynamical quantities at arbitrary frequencies and temperatures. As an application, we determine the spectrum of a quantum dot in an external magnetic field. Furthermore, we discuss magnetic impurities with orbital degeneracy, which have been inferred in recent experiments on quantum dots in an Aharonov-Bohm geometry. It is demonstrated that for spinless electrons, interference between neighbouring levels sets the low-energy scale of the system. Switching on an external field leads to a remarkable crossover into a regime dominated by orbital Kondo screening. We predict that the broadening-induced level splitting should be clearly visible in measurements of the optical absorption power. A more general model including the electron spin is studied within an extended two-band NRG procedure. We observe competition between interference and Kondo screening, similar to the situation in two-impurity models (RKKY).Comment: Invited talk at the DPG spring meeting 2001, to appear in Advances in Solid State Physics 4

Decomposition Based Search - A theoretical and experimental evaluation

In this paper we present and evaluate a search strategy called Decomposition Based Search (DBS) which is based on two steps: subproblem generation and subproblem solution. The generation of subproblems is done through value ranking and domain splitting. Subdomains are explored so as to generate, according to the heuristic chosen, promising subproblems first. We show that two well known search strategies, Limited Discrepancy Search (LDS) and Iterative Broadening (IB), can be seen as special cases of DBS. First we present a tuning of DBS that visits the same search nodes as IB, but avoids restarts. Then we compare both theoretically and computationally DBS and LDS using the same heuristic. We prove that DBS has a higher probability of being successful than LDS on a comparable number of nodes, under realistic assumptions. Experiments on a constraint satisfaction problem and an optimization problem show that DBS is indeed very effective if compared to LDS.Comment: 16 pages, 8 figures. LIA Technical Report LIA00203, University of Bologna, 200