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Title: Atomic bonding effects in annular dark field scanning transmission electron microscopy. II. Experiments

Abstract

Quantitatively calibrated annular dark field scanning transmission electron microscopy (ADF-STEM) imaging experiments were compared to frozen phonon multislice simulations adapted to include chemical bonding effects. Having carefully matched simulation parameters to experimental conditions, a depth-dependent bonding effect was observed for high-angle ADF-STEM imaging of aluminum nitride. This result is explained by computational predictions, systematically examined in the preceding portion of this study, showing the propagation of the converged STEM beam to be highly sensitive to net interatomic charge transfer. Thus, although uncertainties in experimental conditions and simulation accuracy remain, the computationally predicted experimental bonding effect withstands the experimental testing reported here.

Authors:
; ;  [1]
  1. Department of Chemical Engineering and Materials Science, University of Minnesota, Minneapolis, Minnesota 55455 (United States)
Publication Date:
OSTI Identifier:
22592863
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Vacuum Science and Technology. A, Vacuum, Surfaces and Films; Journal Volume: 34; Journal Issue: 4; Other Information: (c) 2016 American Vacuum Society; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING; ACCURACY; ALUMINIUM NITRIDES; BEAMS; BONDING; CHEMICAL BONDS; COMPARATIVE EVALUATIONS; DEPTH; FORECASTING; PHONONS; TESTING; TRANSMISSION ELECTRON MICROSCOPY

Citation Formats

Odlyzko, Michael L., Held, Jacob T., and Mkhoyan, K. Andre, E-mail: mkhoyan@umn.edu. Atomic bonding effects in annular dark field scanning transmission electron microscopy. II. Experiments. United States: N. p., 2016. Web. doi:10.1116/1.4954877.
Odlyzko, Michael L., Held, Jacob T., & Mkhoyan, K. Andre, E-mail: mkhoyan@umn.edu. Atomic bonding effects in annular dark field scanning transmission electron microscopy. II. Experiments. United States. doi:10.1116/1.4954877.
Odlyzko, Michael L., Held, Jacob T., and Mkhoyan, K. Andre, E-mail: mkhoyan@umn.edu. 2016. "Atomic bonding effects in annular dark field scanning transmission electron microscopy. II. Experiments". United States. doi:10.1116/1.4954877.
@article{osti_22592863,
title = {Atomic bonding effects in annular dark field scanning transmission electron microscopy. II. Experiments},
author = {Odlyzko, Michael L. and Held, Jacob T. and Mkhoyan, K. Andre, E-mail: mkhoyan@umn.edu},
abstractNote = {Quantitatively calibrated annular dark field scanning transmission electron microscopy (ADF-STEM) imaging experiments were compared to frozen phonon multislice simulations adapted to include chemical bonding effects. Having carefully matched simulation parameters to experimental conditions, a depth-dependent bonding effect was observed for high-angle ADF-STEM imaging of aluminum nitride. This result is explained by computational predictions, systematically examined in the preceding portion of this study, showing the propagation of the converged STEM beam to be highly sensitive to net interatomic charge transfer. Thus, although uncertainties in experimental conditions and simulation accuracy remain, the computationally predicted experimental bonding effect withstands the experimental testing reported here.},
doi = {10.1116/1.4954877},
journal = {Journal of Vacuum Science and Technology. A, Vacuum, Surfaces and Films},
number = 4,
volume = 34,
place = {United States},
year = 2016,
month = 7
}
  • Annular dark field scanning transmission electron microscopy (ADF-STEM) image simulations were performed for zone-axis-oriented light-element single crystals, using a multislice method adapted to include charge redistribution due to chemical bonding. Examination of these image simulations alongside calculations of the propagation of the focused electron probe reveal that the evolution of the probe intensity with thickness exhibits significant sensitivity to interatomic charge transfer, accounting for observed thickness-dependent bonding sensitivity of contrast in all ADF-STEM imaging conditions. Because changes in image contrast relative to conventional neutral atom simulations scale directly with the net interatomic charge transfer, the strongest effects are seen inmore » crystals with highly polar bonding, while no effects are seen for nonpolar bonding. Although the bonding dependence of ADF-STEM image contrast varies with detector geometry, imaging parameters, and material temperature, these simulations predict the bonding effects to be experimentally measureable.« less
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  • In this report, we show that an annular dark-field detector in an aberration-corrected scanning transmission electron microscope allows the direct observation of light element columns in crystalline lattices. At specific imaging conditions, an enhancement of the intensities of light element columns in the presence of heavy element columns is observed. Experimental results are presented for imaging the nitrogen and carbon atomic columns at the GaN-SiC interface and within the GaN and SiC compounds. The crystal polarity of GaN at the interface is identified. The obtained findings are discussed and are well supported by image simulations.
  • Nanostructure of a ThMoB{sub 4}-type (β-type) TmAlB{sub 4} compound, in which YCrB{sub 4}-type (α-type) domains are locally intergrown, is studied by high-angle annular detector dark-field scanning transmission electron microscopy (HAADF-STEM). Z-contrast images by HAADF-STEM directly represent the arrangements of Tm atoms located at centers of heptagonal atomic columns of B atoms as bright dots, and give us detailed information of intergrowth of type domains in the matrix of the β-type phase, which coherently occurs. Structural and bonding analyses for β-TmAlB{sub 4} point out the closeness in atomic interactions and energy of the α- and β-type structures which support the easymore » formation of such nanostructure intergrowths. From combination between HAADF-STEM and electronic structure calculation, a detailed local crystal structure with intrinsic building defects is effectively revealed. - Graphical abstract: Nanostructure of a ThMoB{sub 4}-type (β-type) TmAlB{sub 4} compound, in which YCrB{sub 4}-type (α-type) domains are locally intergrown, is studied by high-angle annular detector dark-field scanning transmission electron microscopy (HAADF-STEM). Z-contrast images by HAADF-STEM directly represent arrangements of Tm atoms located at centers of heptagonal atomic columns of B atoms as bright dots, and give us detailed information of the characteristic intergrowth structure of type domains in the matrix of the β-type phase. - Highlights: • HAADF-STEM images directly represent arrangements of Tm atoms as bright dots. • The α-type planar domains coherently intergrown in the β-type matrix. • Bright strips appear at overlapped regions of Tm hexagons along interfaces between α- and β-type domains.« less