Signatures of distinct impurity configurations in atomic-resolution valence electron-energy-loss spectroscopy: Application to graphene

Kapetanakis, Myron D.; Oxley, Mark P.; Zhou, Wu; Pennycook, Stephen J.; Idrobo, Juan-Carlos; Pantelides, Sokrates T.

doi:10.1103/PhysRevB.94.155449

Signatures of distinct impurity configurations in atomic-resolution valence electron-energy-loss spectroscopy: Application to graphene

Journal Article · Mon Oct 31 00:00:00 EDT 2016 · Physical Review B

DOI:https://doi.org/10.1103/PhysRevB.94.155449· OSTI ID:1355872

Kapetanakis, Myron D. ^[1]; Oxley, Mark P. ^[2]; Zhou, Wu ^[3]; Pennycook, Stephen J. ^[4]; Idrobo, Juan-Carlos ^[5]; Pantelides, Sokrates T. ^[1]

Vanderbilt Univ., Nashville, TN (United States). Dept. of Physics and Astronomy; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division; Vanderbilt Univ., Nashville, TN (United States). Dept. of Physics and Astronomy
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
National Univ of Singapore (Singapore). Dept. of Materials Science and Engineering
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)

The detection and identification of impurities and other point defects in materials is a challenging task. Signatures for point defects are typically obtained using spectroscopies without spatial resolution. Here in this paper, we demonstrate the power of valence electron-energy-loss spectroscopy (VEELS) in an aberration-corrected scanning transmission-electron microscope (STEM) to provide energy-resolved and atomically resolved maps of electronic excitations of individual impurities which, combined with theoretical simulations, yield unique signatures of distinct bonding configurations of impurities. We report VEELS maps for isolated Si impurities in graphene, which are known to exist in two distinct configurations. We also report simulations of the maps, based on density functional theory and dynamical scattering theory, which agree with and provide direct interpretation of observed features. We show that theoretical VEELS maps exhibit distinct and unambiguous signatures for the threefold- and fourfold-coordinated configurations of Si impurities in different energy-loss windows, corresponding to impurity-induced bound states, resonances, and antiresonances. With the advent of new monochromators and detectors with high energy resolution and low signal-to-noise ratio, the present work ushers an atomically resolved STEM-based spectroscopy of individual impurities as an alternative to conventional spectroscopies for probing impurities and defects.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Vanderbilt Univ., Nashville, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231; AC05-00OR22725; FG02-09ER46554

OSTI ID:: 1355872

Alternate ID(s):: OSTI ID: 1330483
OSTI ID: 1597791

Journal Information:: Physical Review B, Journal Name: Physical Review B Journal Issue: 15 Vol. 94; ISSN 2469-9950; ISSN PRBMDO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Materials Structure, Properties and Dynamics through Scanning Transmission Electron Microscopy Pennycook, Stephen J.; Li, Changjian; Li, Mengsha arXiv https://doi.org/10.48550/arxiv.1908.07238	text	January 2019

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