Signatures of distinct impurity configurations in atomic-resolution valence electron-energy-loss spectroscopy: Application to graphene
Abstract
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.
- Authors:
-
- 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)
- Publication Date:
- Research Org.:
- Vanderbilt Univ., Nashville, TN (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1597791
- Alternate Identifier(s):
- OSTI ID: 1330483; OSTI ID: 1355872
- Grant/Contract Number:
- FG02-09ER46554; AC05-00OR22725; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 94; Journal Issue: 15; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Kapetanakis, Myron D., Oxley, Mark P., Zhou, Wu, Pennycook, Stephen J., Idrobo, Juan-Carlos, and Pantelides, Sokrates T. Signatures of distinct impurity configurations in atomic-resolution valence electron-energy-loss spectroscopy: Application to graphene. United States: N. p., 2016.
Web. doi:10.1103/PhysRevB.94.155449.
Kapetanakis, Myron D., Oxley, Mark P., Zhou, Wu, Pennycook, Stephen J., Idrobo, Juan-Carlos, & Pantelides, Sokrates T. Signatures of distinct impurity configurations in atomic-resolution valence electron-energy-loss spectroscopy: Application to graphene. United States. https://doi.org/10.1103/PhysRevB.94.155449
Kapetanakis, Myron D., Oxley, Mark P., Zhou, Wu, Pennycook, Stephen J., Idrobo, Juan-Carlos, and Pantelides, Sokrates T. Mon .
"Signatures of distinct impurity configurations in atomic-resolution valence electron-energy-loss spectroscopy: Application to graphene". United States. https://doi.org/10.1103/PhysRevB.94.155449. https://www.osti.gov/servlets/purl/1597791.
@article{osti_1597791,
title = {Signatures of distinct impurity configurations in atomic-resolution valence electron-energy-loss spectroscopy: Application to graphene},
author = {Kapetanakis, Myron D. and Oxley, Mark P. and Zhou, Wu and Pennycook, Stephen J. and Idrobo, Juan-Carlos and Pantelides, Sokrates T.},
abstractNote = {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.},
doi = {10.1103/PhysRevB.94.155449},
journal = {Physical Review B},
number = 15,
volume = 94,
place = {United States},
year = {Mon Oct 31 00:00:00 EDT 2016},
month = {Mon Oct 31 00:00:00 EDT 2016}
}
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