Publications (29)59.83 Total impact

 [Show abstract] [Hide abstract]
ABSTRACT: Density function theory (DFT) is the most widely employed electronic structure method because of its favorable scaling with system size and accuracy for a broad range of molecular and condensedphase systems. The advent of massively parallel supercomputers has enhanced the scientific community's ability to study larger system sizes. Groundstate DFT calculations on ∼ 103 valence electrons using traditional algorithms can be routinely performed on presentday supercomputers. The performance characteristics of these massively parallel DFT codes on > 104 computer cores are not well understood. The GPAW code was ported an optimized for the Blue Gene/P architecture. We present our algorithmic parallelization strategy and interpret the results for a number of benchmark test cases.Copyright © 2013 John Wiley & Sons, Ltd.Concurrency and Computation Practice and Experience 12/2013; · 0.85 Impact Factor  [Show abstract] [Hide abstract]
ABSTRACT: We present an implementation of localized atomicorbital basis sets in the projector augmented wave (PAW) formalism within the densityfunctional theory. The implementation in the realspace GPAW code provides a complementary basis set to the accurate but computationally more demanding grid representation. The possibility to switch seamlessly between the two representations implies that simulations employing the local basis can be fine tuned at the end of the calculation by switching to the grid, thereby combining the strength of the two representations for optimal performance. The implementation is tested by calculating atomization energies and equilibrium bulk properties of a variety of molecules and solids, comparing to the grid results. Finally, it is demonstrated how a gridquality structure optimization can be performed with significantly reduced computational effort by switching between the grid and basis representations.Physical review. B, Condensed matter 03/2013; 80(19). · 3.77 Impact Factor  [Show abstract] [Hide abstract]
ABSTRACT: Density functional theory has became the workhorse for simulations of catalytic reactions and computational design of novel catalysis. The generally applied semilocal exchangecorrelation functionals have successfully predicted catalytic reaction trends over a variety of surfaces. However, in order to achieve quantitative predictions of reaction rates for moleculesurface systems, in particular where there is weak Van der Waals interactions or strong correlation, it is of vital importance to include nonlocal correlation effects. The use of random phase approximation (RPA) to construct the correlation energy, combined with the exact, selfinteraction free exchange energy, offers a nonempirical way for accurately describe the adsorption energies [1] and dispersion forces [2]. We have recently implemented RPA in the GPAW code [34], an electronic structure package using projector augmented wave method and real space grids. In this talk I will present our initial results comparing RPA and generalized gradient functionals for the activation energies and reaction energies for transition metal or metal oxide surfaces. [4pt] [1] L. Schimka, et.al, Nature Mat. 9, 741 (2010) [2] T. Olsen, et.al, Phys. Rev. Lett. 107, 156401 (2011) [3] J. Yan, et.al, Phys. Rev. B 83, 245122 (2011). [4] J. Yan, et.al, Phys. Rev. Lett. 106, 146803 (2011)02/2012; 
Article: GPAW on Blue Gene/P
[Show abstract] [Hide abstract]
ABSTRACT: Density function theory (DFT) is the most widely employed electronic structure method due to its favorable scaling with system size and accuracy for a broad range of molecular and condensedphase systems. The advent of massively parallel supercomputers have enhanced the scientific community's ability to study larger system sizes. Ground state DFT calculations of systems with O(10^3) valence electrons can be routinely performed on presentday supercomputers. The performance of these massively parallel DFT codes at the scale of 1  10K execution threads are not well understood; even experienced DFT users are unaware of Amdahl's Law and the nontrivial scaling bottlenecks that are present in standard O(N^3) DFT algorithms. The GPAW code was ported an optimized for the Blue Gene/P. We present our algorithmic parallelization strategy and interpret the results for a number of benchmark tests cases. Lastly, I will describe opportunities for computer allocations at the Argonne Leadership Computing Facility.03/2011;  [Show abstract] [Hide abstract]
ABSTRACT: AbstractWe address the fundamental question of which size a metallic nanoparticle needs to have before its surface chemical properties can be considered to be those of a solid, rather than those of a large molecule. Calculations of adsorption energies for carbon monoxide and oxygen on a series of gold nanoparticles ranging from 13 to 1,415 atoms, or 0.8–3.7nm, have been made possible by exploiting massively parallel computing on up to 32,768 cores on the Blue Gene/P computer at Argonne National Laboratory. We show that bulk surface properties are obtained for clusters larger than ca. 560 atoms (2.7nm). Below that critical size, finitesize effects can be observed, and we show those to be related to variations in the local atomic structure augmented by quantum size effects for the smallest clusters. Graphical Abstract KeywordsNanoparticle–Size effects–DFTCatalysis Letters 01/2011; 141(8):10671071. · 2.24 Impact Factor  [Show abstract] [Hide abstract]
ABSTRACT: We describe the implementation of Kshell core level spectroscopies (Xray absorption (XAS), Xray emission (XES), and Xray photoemission (XPS)) in the realspacegridbased Projector Augmented Wave (PAW) GPAW code. The implementation for XAS is based on the Haydock recursion method avoiding computation of unoccupied states. The absolute energy scale is computed with the Delta Kohn–Sham method which is possible using specific PAW setups for the corehole states. We show computed spectra for selected test cases (gas phase H2O and bulk diamond) and discuss the dependence on grid spacing and box size. In the case of diamond we include vibrational effects by sampling spectra from the ground state vibrational distribution and discuss the importance of those effects for the experimentally observed features. We apply the method to XPS, XES and XAS of CO adsorbed on Ni(100) and compare to experimental data where possible.Fuel and Energy Abstracts 01/2011; 184(8):427439.  [Show abstract] [Hide abstract]
ABSTRACT: Electronic structure calculations have become an indispensable tool in many areas of materials science and quantum chemistry. Even though the KohnSham formulation of the densityfunctional theory (DFT) simplifies the manybody problem significantly, one is still confronted with several numerical challenges. In this article we present the projector augmentedwave (PAW) method as implemented in the GPAW program package (https://wiki.fysik.dtu.dk/gpaw) using a uniform realspace grid representation of the electronic wavefunctions. Compared to more traditional plane wave or localized basis set approaches, realspace grids offer several advantages, most notably good computational scalability and systematic convergence properties. However, as a unique feature GPAW also facilitates a localized atomicorbital basis set in addition to the grid. The efficient atomic basis set is complementary to the more accurate grid, and the possibility to seamlessly switch between the two representations provides great flexibility. While DFT allows one to study ground state properties, timedependent densityfunctional theory (TDDFT) provides access to the excited states. We have implemented the two common formulations of TDDFT, namely the linearresponse and the time propagation schemes. Electron transport calculations under finitebias conditions can be performed with GPAW using nonequilibrium Green functions and the localized basis set. In addition to the basic features of the realspace PAW method, we also describe the implementation of selected exchangecorrelation functionals, parallelization schemes, ΔSCFmethod, xray absorption spectra, and maximally localized Wannier orbitals.Journal of Physics Condensed Matter 06/2010; 22(25):253202. · 2.22 Impact Factor  [Show abstract] [Hide abstract]
ABSTRACT: We use density functional theory (DFT) with a recently developed van der Waals density functional (vdWDF) to study the adsorption of graphene on Al, Cu, Ag, Au, Pt, Pd, Co and Ni(111) surfaces. In constrast to the local density approximation (LDA) which predicts relatively strong binding for Ni,Co and Pd, the vdWDF predicts weak binding for all metals and metalgraphene distances in the range 3.403.72 \AA. At these distances the graphene bandstructure as calculated with DFT and the manybody G$_0$W$_0$ method is basically unaffected by the substrate, in particular there is no opening of a band gap at the $K$point. Comment: 4 pages, 3 figuresPhysical review. B, Condensed matter 12/2009; · 3.77 Impact Factor  [Show abstract] [Hide abstract]
ABSTRACT: We present a computational screening study of ternary metal borohydrides for reversible hydrogen storage based on density functional theory. We investigate the stability and decomposition of alloys containing 1 alkali metal atom, Li, Na, or K (M(1)); and 1 alkali, alkaline earth or 3d/4d transition metal atom (M(2)) plus two to five (BH(4))() groups, i.e., M(1)M(2)(BH(4))(25), using a number of model structures with trigonal, tetrahedral, octahedral, and free coordination of the metal borohydride complexes. Of the over 700 investigated structures, about 20 were predicted to form potentially stable alloys with promising decomposition energies. The M(1)(Al/Mn/Fe)(BH(4))(4), (Li/Na)Zn(BH(4))(3), and (Na/K)(Ni/Co)(BH(4))(3) alloys are found to be the most promising, followed by selected M(1)(Nb/Rh)(BH(4))(4) alloys.The Journal of Chemical Physics 08/2009; 131(1):014101. · 3.12 Impact Factor  Physical Review B (Condensed Matter and Materials Physics). 01/2009; 80(19):195112.
 [Show abstract] [Hide abstract]
ABSTRACT: We present a practical scheme for performing error estimates for densityfunctional theory calculations. The approach, which is based on ideas from Bayesian statistics, involves creating an ensemble of exchangecorrelation functionals by comparing with an experimental database of binding energies for molecules and solids. Fluctuations within the ensemble can then be used to estimate errors relative to experiment on calculated quantities such as binding energies, bond lengths, and vibrational frequencies. It is demonstrated that the error bars on energy differences may vary by orders of magnitude for different systems in good agreement with existing experience.Physical Review Letters 12/2005; 95(21):216401. · 7.73 Impact Factor  [Show abstract] [Hide abstract]
ABSTRACT: A gridbased realspace implementation of the Projector Augmented Wave (PAW) method of P. E. Blochl [Phys. Rev. B 50, 17953 (1994)] for Density Functional Theory (DFT) calculations is presented. The use of uniform 3D realspace grids for representing wave functions, densities and potentials allows for flexible boundary conditions, efficient multigrid algorithms for solving Poisson and KohnSham equations, and efficient parallelization using simple realspace domaindecomposition. We use the PAW method to perform allelectron calculations in the frozen core approximation, with smooth valence wave functions that can be represented on relatively coarse grids. We demonstrate the accuracy of the method by calculating the atomization energies of twenty small molecules, and the bulk modulus and lattice constants of bulk aluminum. We show that the approach in terms of computational efficiency is comparable to standard planewave methods, but the memory requirements are higher. Comment: 13 pages, 3 figures, accepted for publication in Physical Review BPhysical review. B, Condensed matter 11/2004; · 3.77 Impact Factor  Physical Review B (Condensed Matter and Materials Physics). 01/2004; 69(21):214104.
 [Show abstract] [Hide abstract]
ABSTRACT: The quasicontinuum method is a way of reducing the number of degrees of freedom in an atomistic simulation by removing the majority of the atoms in regions of slowly varying strain fields. Due to the different ways the energy of the atoms is calculated in the coarsegrained regions and the regions where all the atoms are present, unphysical forces called “ghost forces” arise at the interfaces. Corrections may be used to almost remove the ghost forces, but the correction forces are nonconservative, ruining energy conservation in dynamic simulations. We show that it is possible to formulate the quasicontinuum method without these problems by introducing a buffer layer between the two regions of space. The method is applicable to shortranged potentials in the facecentered cubic, bodycentered cubic, and hexagonal closepacked crystal structures.Physical Review B 01/2004; 69(21). · 3.66 Impact Factor 
Conference Paper: The Quasicontinuum Method Revisited
Proceedings; 01/2002  [Show abstract] [Hide abstract]
ABSTRACT: The diffusion of individual N adatoms on Fe(100) has been studied using scanning tunneling microscopy and ab initio density functional theory (DFT) calculations. The measured diffusion barrier for isolated N adatoms is E(d) = (0.92+/0.04) eV, with a prefactor of nu(0) = 4.3x10(12) s(1), which is in quantitative agreement with the DFT calculations. The diffusion is strongly coupled to lattice distortions, and, as a consequence, the presence of other N adatoms introduces an anisotropy in the diffusion. Based on experimentally determined values of the diffusion barriers and adsorbateadsorbate interactions, the potential energy surface experienced by a N adatom is determined.Physical Review Letters 06/2000; 84(21):4898901. · 7.73 Impact Factor  [Show abstract] [Hide abstract]
ABSTRACT: We report extensive density functional calculations of the energetics of N2adsorption and dissociation on a Fe(111) surface. From the calculations we can present a detailed picture of the rate limiting step in the ammonia synthesis which is consistent with available experimental observations. Four different molecularly adsorbed states are identified, including a new state not seen by experiment. The new state is the true precursor to dissociation. We find that there are two dissociation channels, one going through all the molecular states sequentially with a low energy barrier, but a high entropy barrier, and the other a direct channel into the new precursor, which is highly activated. In this way we can explain both the measured sticking probability for a thermal gas of N2above a Fe(111) surface and the molecular beam scattering experiments. During ammonia synthesis conditions the low barrier channel is expected to dominate, but at the highest synthesis temperatures, the high barrier channels may become the most effective. The origin of the alkali promotion of the N2dissociation process is also discussed.Journal of Catalysis  J CATAL. 01/1999; 182(2):479488.  [Show abstract] [Hide abstract]
ABSTRACT: Adsorption energies and structures for N atoms on three lowindex surfaces of Fe have been calculated using density functional theory (DFT) and the generalized gradient approximation (GGA). At low N coverage the adsorption energy on Fe(100) is found to be ∼0.7eV higher than on the (111) and (110) surfaces – particularly the c(2×2)N/Fe(100) structure with the N atoms in fourfold sites is very stable. We attribute the differences in adsorption energy to the lack of fourfold sites on the (111) and (110) surfaces. We suggest that at higher N coverages, islands with a structure similar to the c(2×2)N/Fe(100) structure will form on the (111) and (110) surfaces.Surface Science 01/1999; 422(1):816. · 1.84 Impact Factor  Surface Science  SURFACE SCI. 01/1998; 400(1):290313.
Publication Stats
585  Citations  
59.83  Total Impact Points  
Top Journals
Institutions

1997–2013

Technical University of Denmark
 • Center for Atomicscale Materials Design
 • Department of Physics
Copenhagen, Capital Region, Denmark


2011

Stanford University
Palo Alto, California, United States


2010

CSCIT Center for Science Ltd
Esbo, Southern Finland Province, Finland


2000

Aarhus University
 Department of Physics and Astronomy
Århus, Central Jutland, Denmark
