Simulation of electron energy loss spectra of nanomaterials with linear-scaling density functional theory

Tait, E. W.; Ratcliff, L. E.; Payne, M. C.; Haynes, P. D.; Hine, N. D. M.

doi:10.1088/0953-8984/28/19/195202

Title: Simulation of electron energy loss spectra of nanomaterials with linear-scaling density functional theory

Journal Article · Wed Apr 20 00:00:00 EDT 2016 · Journal of Physics. Condensed Matter

DOI:https://doi.org/10.1088/0953-8984/28/19/195202· OSTI ID:1248244

Tait, E. W.; Ratcliff, L. E.; Payne, M. C.; Haynes, P. D.; Hine, N. D. M.

Experimental techniques for electron energy loss spectroscopy (EELS) combine high energy resolution with high spatial resolution. They are therefore powerful tools for investigating the local electronic structure of complex systems such as nanostructures, interfaces and even individual defects. Interpretation of experimental electron energy loss spectra is often challenging and can require theoretical modelling of candidate structures, which themselves may be large and complex, beyond the capabilities of traditional cubic-scaling density functional theory. In this work, we present functionality to compute electron energy loss spectra within the onetep linear-scaling density functional theory code. We first demonstrate that simulated spectra agree with those computed using conventional plane wave pseudopotential methods to a high degree of precision. The ability of onetep to tackle large problems is then exploited to investigate convergence of spectra with respect to supercell size. As a result, we apply the novel functionality to a study of the electron energy loss spectra of defects on the (1 0 1) surface of an anatase slab and determine concentrations of defects which might be experimentally detectable.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE; Argonne National Laboratory - Argonne Leadership Computing Facility

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1248244

Alternate ID(s):: OSTI ID: 1248245; OSTI ID: 1275830

Journal Information:: Journal of Physics. Condensed Matter, Journal Name: Journal of Physics. Condensed Matter Vol. 28 Journal Issue: 19; ISSN 0953-8984

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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Cited by: 15 works

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References (33)

Hybrid MPI-OpenMP Parallelism in the ONETEP Linear-Scaling Electronic Structure Code: Application to the Delamination of Cellulose Nanofibrils Wilkinson, Karl A.; Hine, Nicholas D. M.; Skylaris, Chris-Kriton Journal of Chemical Theory and Computation, Vol. 10, Issue 11 https://doi.org/10.1021/ct500686r	journal	October 2014
Site dependence and peak assignment of $Y {Ba}_{2} {Cu}_{3} O_{7 - x}$ O $K$ -edge electron energy loss near-edge fine structure Mizoguchi, Teruyasu; Varela, Maria; Buban, James P. Physical Review B, Vol. 77, Issue 2 https://doi.org/10.1103/PhysRevB.77.024504	journal	January 2008
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Theory of core-hole effects in $1 s$ core-level spectroscopy of the first-row elements Gao, Shang-Peng; Pickard, Chris J.; Payne, Mike C. Physical Review B, Vol. 77, Issue 11 https://doi.org/10.1103/PhysRevB.77.115122	journal	March 2008
ELNES study of carbon K-edge spectra of plasma deposited carbon films Hamon, Ann-Lenaig; Verbeeck, Jo; Schryvers, Dominique Journal of Materials Chemistry, Vol. 14, Issue 13 https://doi.org/10.1039/b406468m	journal	January 2004
First-principles calculations of ELNES and XANES of selected wide-gap materials: Dependence on crystal structure and orientation Mizoguchi, Teruyasu; Tanaka, Isao; Yoshioka, Satoru Physical Review B, Vol. 70, Issue 4 https://doi.org/10.1103/PhysRevB.70.045103	journal	July 2004
Generation of Projector Augmented-Wave atomic data: A 71 element validated table in the XML format Jollet, François; Torrent, Marc; Holzwarth, Natalie Computer Physics Communications, Vol. 185, Issue 4 https://doi.org/10.1016/j.cpc.2013.12.023	journal	April 2014
A “Thickness Series”: Weak Signal Extraction of ELNES in EELS Spectra From Surfaces Zhu, Guo-zhen; Botton, Gianluigi A. Microscopy and Microanalysis, Vol. 20, Issue 3 https://doi.org/10.1017/S1431927613013676	journal	December 2013
Crystal Structure of the ZrO Phase at Zirconium/Zirconium Oxide Interfaces: Crystal Structure of the ZrO Phase … Nicholls, Rebecca J.; Ni, Na; Lozano-Perez, Sergio Advanced Engineering Materials, Vol. 17, Issue 2 https://doi.org/10.1002/adem.201400133	journal	June 2014
Sr ₂ MgMoO ₆ _- _δ : Structure, Phase Stability, and Cation Site Order Control of Reduction Bernuy-Lopez, Carlos; Allix, Mathieu; Bridges, Craig A. Chemistry of Materials, Vol. 19, Issue 5 https://doi.org/10.1021/cm0624116	journal	March 2007
Calculating optical absorption spectra for large systems using linear-scaling density functional theory Ratcliff, Laura E.; Hine, Nicholas D. M.; Haynes, Peter D. Physical Review B, Vol. 84, Issue 16 https://doi.org/10.1103/PhysRevB.84.165131	journal	October 2011
Toward reliable density functional methods without adjustable parameters: The PBE0 model Adamo, Carlo; Barone, Vincenzo The Journal of Chemical Physics, Vol. 110, Issue 13 https://doi.org/10.1063/1.478522	journal	April 1999
Inhomogeneous Electron Gas Hohenberg, P.; Kohn, W. Physical Review, Vol. 136, Issue 3B, p. B864-B871 https://doi.org/10.1103/PhysRev.136.B864	journal	November 1964
Near-edge structure in electron-energy-loss spectra of MgO Lindner, Th.; Sauer, H.; Engel, W. Physical Review B, Vol. 33, Issue 1 https://doi.org/10.1103/PhysRevB.33.22	journal	January 1986
Grain boundary bonding state and fracture energy in small amount of oxide-doped fine-grained Al2O3 Takigawa, Y.; Ikuhara, Y.; Sakuma, T. Journal of Materials Science, Vol. 34, Issue 9, p. 1991-1997 https://doi.org/10.1023/A:1004574702475	journal	January 1999
The United Kingdom Chemical Database Service Fletcher, David A.; McMeeking, Robert F.; Parkin, Donald Journal of Chemical Information and Computer Sciences, Vol. 36, Issue 4 https://doi.org/10.1021/ci960015+	journal	January 1996
Core-Level Spectroscopy to Probe the Oxidation State of Single Europium Atoms Tizei, Luiz H. G.; Nakanishi, Ryo; Kitaura, Ryo Physical Review Letters, Vol. 114, Issue 19 https://doi.org/10.1103/PhysRevLett.114.197602	journal	May 2015
E9: The New High-Resolution Neutron Powder Diffractometer at the Berlin Neutron Scattering Center Többens, D. M.; Stüßer, N.; Knorr, K. Materials Science Forum, Vol. 378-381 https://doi.org/10.4028/www.scientific.net/MSF.378-381.288	journal	October 2001
Structure of graphite by neutron diffraction Trucano, Peter; Chen, Ruey Nature, Vol. 258, Issue 5531 https://doi.org/10.1038/258136a0	journal	November 1975
First principles pseudopotential calculation of electron energy loss near edge structures of lattice imperfections Mizoguchi, Teruyasu; Matsunaga, Katsuyuki; Tochigi, Eita Micron, Vol. 43, Issue 1 https://doi.org/10.1016/j.micron.2011.07.005	journal	January 2012
Mapping functional groups on oxidised multi-walled carbon nanotubes at the nanometre scale Goode, A. E.; Hine, N. D. M.; Chen, S. Chem. Commun., Vol. 50, Issue 51 https://doi.org/10.1039/c4cc02026j	journal	January 2014
XANES and ELNES in Ceramic Science: XANES and ELNES in Ceramic Science Tanaka, Isao; Mizoguchi, Teruyasu; Yamamoto, Tomoyuki Journal of the American Ceramic Society, Vol. 88, Issue 8 https://doi.org/10.1111/j.1551-2916.2005.00547.x	journal	July 2005
Achieving plane wave accuracy in linear-scaling density functional theory applied to periodic systems: A case study on crystalline silicon Skylaris, Chris-Kriton; Haynes, Peter D. The Journal of Chemical Physics, Vol. 127, Issue 16 https://doi.org/10.1063/1.2796168	journal	October 2007
Structure of chemically derived mono- and few-atomic-layer boron nitride sheets Han, Wei-Qiang; Wu, Lijun; Zhu, Yimei Applied Physics Letters, Vol. 93, Issue 22 https://doi.org/10.1063/1.3041639	journal	December 2008
Sparsity of the Density Matrix in Kohn-Sham Density Functional Theory and an Assessment of Linear System-Size Scaling Methods Baer, Roi; Head-Gordon, Martin Physical Review Letters, Vol. 79, Issue 20 https://doi.org/10.1103/PhysRevLett.79.3962	journal	November 1997
Introducing ONETEP : Linear-scaling density functional simulations on parallel computers Skylaris, Chris-Kriton; Haynes, Peter D.; Mostofi, Arash A. The Journal of Chemical Physics, Vol. 122, Issue 8 https://doi.org/10.1063/1.1839852	journal	February 2005
Density Functional and Density Matrix Method Scaling Linearly with the Number of Atoms Kohn, W. Physical Review Letters, Vol. 76, Issue 17 https://doi.org/10.1103/PhysRevLett.76.3168	journal	April 1996
First principles methods using CASTEP Clark, Stewart J.; Segall, Matthew D.; Pickard, Chris J. Zeitschrift für Kristallographie - Crystalline Materials, Vol. 220, Issue 5/6 https://doi.org/10.1524/zkri.220.5.567.65075	journal	January 2005
Error Estimates for Solid-State Density-Functional Theory Predictions: An Overview by Means of the Ground-State Elemental Crystals Lejaeghere, K.; Van Speybroeck, V.; Van Oost, G. Critical Reviews in Solid State and Materials Sciences, Vol. 39, Issue 1 https://doi.org/10.1080/10408436.2013.772503	journal	October 2013
Hydrogenated K ₄ carbon: A new stable cubic gauche structure of carbon hydride Lian, Chao-Sheng; Wang, Xin-Quan; Wang, Jian-Tao The Journal of Chemical Physics, Vol. 138, Issue 2 https://doi.org/10.1063/1.4773584	journal	January 2013
Comparison of the electronic structure of anatase and rutile ${TiO}_{2}$ single-crystal surfaces using resonant photoemission and x-ray absorption spectroscopy Thomas, A. G.; Flavell, W. R.; Mallick, A. K. Physical Review B, Vol. 75, Issue 3 https://doi.org/10.1103/PhysRevB.75.035105	journal	January 2007
Probing the Bonding and Electronic Structure of Single Atom Dopants in Graphene with Electron Energy Loss Spectroscopy Ramasse, Quentin M.; Seabourne, Che R.; Kepaptsoglou, Despoina-Maria Nano Letters, Vol. 13, Issue 10 https://doi.org/10.1021/nl304187e	journal	January 2013
Self-Consistent Equations Including Exchange and Correlation Effects Kohn, W.; Sham, L. J. Physical Review, Vol. 140, Issue 4A, p. A1133-A1138 https://doi.org/10.1103/PhysRev.140.A1133	journal	November 1965

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36 MATERIALS SCIENCE
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Title: Simulation of electron energy loss spectra of nanomaterials with linear-scaling density functional theory

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