Title: Low-loss electron energy loss spectroscopy: An atomic-resolution complement to optical spectroscopies and application to graphene

Abstract

Photon-based spectroscopies have played a central role in exploring the electronic properties of crystalline solids and thin films. Though they remain a powerful tool for probing the electronic properties of nanostructures, they are limited by lack of spatial resolution. On the other hand, electron-based spectroscopies, e.g., electron energy loss spectroscopy (EELS), are now capable of subangstrom spatial resolution. Core-loss EELS, a spatially resolved analog of x-ray absorption, has been used extensively in the study of inhomogeneous complex systems. In this paper, we demonstrate that low-loss EELS in an aberration-corrected scanning transmission electron microscope, which probes low-energy excitations, combined with a theoretical framework for simulating and analyzing the spectra, is a powerful tool to probe low-energy electron excitations with atomic-scale resolution. The theoretical component of the method combines density functional theory–based calculations of the excitations with dynamical scattering theory for the electron beam. We apply the method to monolayer graphene in order to demonstrate that atomic-scale contrast is inherent in low-loss EELS even in a perfectly periodic structure. The method is a complement to optical spectroscopy as it probes transitions entailing momentum transfer. The theoretical analysis identifies the spatial and orbital origins of excitations, holding the promise of ultimately becoming amore » powerful probe of the structure and electronic properties of individual point and extended defects in both crystals and inhomogeneous complex nanostructures. The method can be extended to probe magnetic and vibrational properties with atomic resolution.« less

Authors:

Kapetanakis, Myron ^[1]; Zhou, Wu ^[2]; Oxley, Mark P. ^[1]; Lee, Jaekwang ^[3]; Prange, Micah P. ^[4]; Pennycook, Stephen J. ^[5]; Idrobo Tapia, Juan Carlos ^[2]; Pantelides, Sokrates T. ^[1]

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+ Show Author Affiliations

1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Vanderbilt Univ., Nashville, TN (United States)
2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Pusan National Univ. (Korea)
4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
5. Univ. of Tennessee, Knoxville, TN (United States); National Univ. of Singapore (Singapore)

Publication Date:

Fri Sep 25 00:00:00 EDT 2015

Research Org.:

Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science; Vanderbilt Univ., Nashville, TN (United States); University of California, Berkeley, CA (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1223067

Alternate Identifier(s):

OSTI ID: 1224631; OSTI ID: 1597697

Grant/Contract Number:  

AC05-00OR22725; FG02-09ER46554; AC02-05CH11231

Resource Type:

Accepted Manuscript

Journal Name:

Physical Review. B, Condensed Matter and Materials Physics

Additional Journal Information:

Journal Volume: 92; Journal Issue: 12; Journal ID: ISSN 1098-0121

Publisher:

American Physical Society (APS)

Country of Publication:

United States

Language:

English

Subject:

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY