Measurement Error in Atomic-Scale Scanning Transmission Electron Microscopy—Energy-Dispersive X-Ray Spectroscopy (STEM-EDS) Mapping of a Model Oxide Interface

Spurgeon, Steven R.; Du, Yingge; Chambers, Scott A.

doi:10.1017/S1431927617000368

Measurement Error in Atomic-Scale Scanning Transmission Electron Microscopy—Energy-Dispersive X-Ray Spectroscopy (STEM-EDS) Mapping of a Model Oxide Interface

Journal Article · Wed Apr 05 00:00:00 EDT 2017 · Microscopy and Microanalysis

DOI:https://doi.org/10.1017/S1431927617000368· OSTI ID:1355453

; Du, Yingge; Chambers, Scott A.

Abstract

With the development of affordable aberration correctors, analytical scanning transmission electron microscopy (STEM) studies of complex interfaces can now be conducted at high spatial resolution at laboratories worldwide. Energy-dispersive X-ray spectroscopy (EDS) in particular has grown in popularity, as it enables elemental mapping over a wide range of ionization energies. However, the interpretation of atomically resolved data is greatly complicated by beam–sample interactions that are often overlooked by novice users. Here we describe the practical factors—namely, sample thickness and the choice of ionization edge—that affect the quantification of a model perovskite oxide interface. Our measurements of the same sample, in regions of different thickness, indicate that interface profiles can vary by as much as 2–5 unit cells, depending on the spectral feature. This finding is supported by multislice simulations, which reveal that on-axis maps of even perfectly abrupt interfaces exhibit significant delocalization. Quantification of thicker samples is further complicated by channeling to heavier sites across the interface, as well as an increased signal background. We show that extreme care must be taken to prepare samples to minimize channeling effects and argue that it may not be possible to extract atomically resolved information from many chemical maps.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

Contributing Organization:: EDS; STEM; interfaces; multislice; oxides

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1355453

Alternate ID(s):: OSTI ID: 1361980

Report Number(s):: PNNL-SA--119131

Journal Information:: Microscopy and Microanalysis, Journal Name: Microscopy and Microanalysis Journal Issue: 03 Vol. 23; ISSN 1431-9276; ISSN applab

Publisher:: Microscopy Society of America (MSA)Copyright Statement

Country of Publication:: United States

Language:: English

References (24)

Perovskite Sr-Doped LaCrO ₃ as a New p-Type Transparent Conducting Oxide Zhang, Kelvin H. L.; Du, Yingge; Papadogianni, Alexandra Advanced Materials, Vol. 27, Issue 35 https://doi.org/10.1002/adma.201501959	journal	August 2015
Advances in the growth and characterization of magnetic, ferroelectric, and multiferroic oxide thin films Martin, L. W.; Chu, Y. -H.; Ramesh, R. Materials Science and Engineering: R: Reports, Vol. 68, Issue 4-6 https://doi.org/10.1016/j.mser.2010.03.001	journal	May 2010
An electron microscope for the aberration-corrected era Krivanek, O. L.; Corbin, G. J.; Dellby, N. Ultramicroscopy, Vol. 108, Issue 3 https://doi.org/10.1016/j.ultramic.2007.07.010	journal	February 2008
Modelling the inelastic scattering of fast electrons Allen, L. J.; D׳Alfonso, A. J.; Findlay, S. D. Ultramicroscopy, Vol. 151 https://doi.org/10.1016/j.ultramic.2014.10.011	journal	April 2015
On the quantitativeness of EDS STEM Lugg, N. R.; Kothleitner, G.; Shibata, N. Ultramicroscopy, Vol. 151 https://doi.org/10.1016/j.ultramic.2014.11.029	journal	April 2015
Energy dispersive X-ray analysis on an absolute scale in scanning transmission electron microscopy Chen, Z.; D'Alfonso, A. J.; Weyland, M. Ultramicroscopy, Vol. 157 https://doi.org/10.1016/j.ultramic.2015.05.010	journal	October 2015
Quantitative atomic resolution elemental mapping via absolute-scale energy dispersive X-ray spectroscopy Chen, Z.; Weyland, M.; Sang, X. Ultramicroscopy, Vol. 168 https://doi.org/10.1016/j.ultramic.2016.05.008	journal	September 2016
Challenges to Quantitative Multivariate Statistical Analysis of Atomic-Resolution X-Ray Spectral Kotula, Paul G.; Klenov, Dmitri O.; von Harrach, H. Sebastian Microscopy and Microanalysis, Vol. 18, Issue 4 https://doi.org/10.1017/S1431927612001201	journal	July 2012
Chemical Quantification of Atomic-Scale EDS Maps under Thin Specimen Conditions Lu, Ping; Romero, Eric; Lee, Shinbuhm Microscopy and Microanalysis, Vol. 20, Issue 6 https://doi.org/10.1017/S1431927614013245	journal	October 2014
Why some interfaces cannot be sharp Nakagawa, Naoyuki; Hwang, Harold Y.; Muller, David A. Nature Materials, Vol. 5, Issue 3, p. 204-209 https://doi.org/10.1038/nmat1569	journal	January 2006
Atomic-scale chemical quantification of oxide interfaces using energy-dispersive X-ray spectroscopy Lu, Ping; Xiong, Jie; Van Benthem, Mark Applied Physics Letters, Vol. 102, Issue 17 https://doi.org/10.1063/1.4804184	journal	April 2013
Misfit strain driven cation inter-diffusion across an epitaxial multiferroic thin film interface Sankara Rama Krishnan, P. S.; Morozovska, Anna N.; Eliseev, Eugene A. Journal of Applied Physics, Vol. 115, Issue 5 https://doi.org/10.1063/1.4862556	journal	February 2014
Interpreting atomic-resolution spectroscopic images Oxley, M. P.; Varela, M.; Pennycook, T. J. Physical Review B, Vol. 76, Issue 6 https://doi.org/10.1103/PhysRevB.76.064303	journal	August 2007
Atomic-resolution chemical mapping using energy-dispersive x-ray spectroscopy D’Alfonso, A. J.; Freitag, B.; Klenov, D. Physical Review B, Vol. 81, Issue 10 https://doi.org/10.1103/PhysRevB.81.100101	journal	March 2010
Quantum mechanical model for phonon excitation in electron diffraction and imaging using a Born-Oppenheimer approximation Forbes, B. D.; Martin, A. V.; Findlay, S. D. Physical Review B, Vol. 82, Issue 10 https://doi.org/10.1103/PhysRevB.82.104103	journal	September 2010
Contribution of thermally scattered electrons to atomic resolution elemental maps Forbes, B. D.; D'Alfonso, A. J.; Williams, R. E. A. Physical Review B, Vol. 86, Issue 2 https://doi.org/10.1103/PhysRevB.86.024108	journal	July 2012
Cation intermixing and electronic deviations at the insulating LaCrO 3 /SrTiO 3 (001) interface Colby, R.; Qiao, L.; Zhang, K. H. L. Physical Review B, Vol. 88, Issue 15 https://doi.org/10.1103/PhysRevB.88.155325	journal	October 2013
Contrast Reversal in Atomic-Resolution Chemical Mapping Wang, P.; D’Alfonso, A. J.; Findlay, S. D. Physical Review Letters, Vol. 101, Issue 23 https://doi.org/10.1103/PhysRevLett.101.236102	journal	December 2008
Quantitative Elemental Mapping at Atomic Resolution Using X-Ray Spectroscopy Kothleitner, G.; Neish, M. J.; Lugg, N. R. Physical Review Letters, Vol. 112, Issue 8 https://doi.org/10.1103/PhysRevLett.112.085501	journal	February 2014
Local Observation of the Site Occupancy of Mn in a MnFePSi Compound Neish, M. J.; Oxley, M. P.; Guo, J. Physical Review Letters, Vol. 114, Issue 10 https://doi.org/10.1103/PhysRevLett.114.106101	journal	March 2015
Colloquium : Emergent properties in plane view: Strong correlations at oxide interfaces Chakhalian, Jak; Freeland, John W.; Millis, Andrew J. Reviews of Modern Physics, Vol. 86, Issue 4 https://doi.org/10.1103/RevModPhys.86.1189	journal	October 2014
Atomic-Scale Chemical Imaging of Composition and Bonding by Aberration-Corrected Microscopy Muller, D. A.; Kourkoutis, L. F.; Murfitt, M. Science, Vol. 319, Issue 5866 https://doi.org/10.1126/science.1148820	journal	February 2008
Oxide Interfaces--An Opportunity for Electronics Mannhart, J.; Schlom, D. G. Science, Vol. 327, Issue 5973, p. 1607-1611 https://doi.org/10.1126/science.1181862	journal	March 2010
Chemical mapping at atomic resolution using energy-dispersive x-ray spectroscopy Allen, Leslie J.; D’Alfonso, Adrian J.; Freitag, Bert MRS Bulletin, Vol. 37, Issue 1 https://doi.org/10.1557/mrs.2011.331	journal	January 2012

Cited By (7)

Electronic Structure and Band Alignment of LaMnO ₃ /SrTiO ₃ Polar/Nonpolar Heterojunctions Kaspar, Tiffany C.; Sushko, Peter V.; Spurgeon, Steven R. Advanced Materials Interfaces, Vol. 6, Issue 1 https://doi.org/10.1002/admi.201801428	journal	November 2018
High-temperature superconductivity at the lanthanum cuprate/lanthanum–strontium nickelate interface Baiutti, F.; Gregori, G.; Suyolcu, Y. E. Nanoscale, Vol. 10, Issue 18 https://doi.org/10.1039/c8nr00885j	journal	January 2018
Atomic-scale mapping of interface reconstructions in multiferroic heterostructures Huang, Weichuan; Yin, Yuewei; Li, Xiaoguang Applied Physics Reviews, Vol. 5, Issue 4 https://doi.org/10.1063/1.5053426	journal	December 2018
Impact of growth kinetics on the interface morphology and magnetization in La _1/3 Sr _2/3 FeO ₃ /La _2/3 Sr _1/3 MnO ₃ heterostructures Waschk, M.; Sarkar, A.; Barthel, J. Journal of Physics: Condensed Matter, Vol. 32, Issue 16 https://doi.org/10.1088/1361-648x/ab678c	journal	January 2020
Digital modulation of the nickel valence state in a cuprate-nickelate heterostructure Wrobel, F.; Geisler, B.; Wang, Y. Physical Review Materials, Vol. 2, Issue 3 https://doi.org/10.1103/physrevmaterials.2.035001	journal	March 2018
Impact of growth kinetics on the interface morphology and magnetization in La 1/3 Sr 2/3 FeO 3 /La 2/3 Sr 1/3 MnO 3 heterostructures Waschk, M.; Sarkar, A.; Barthel, J. RWTH Aachen University https://doi.org/10.18154/rwth-2020-00983	text	January 2020
Digital modulation of the nickel valence state in a cuprate-nickelate heterostructure Wrobel, F.; Geisler, B.; Wang, Y. arXiv https://doi.org/10.48550/arxiv.1706.02173	text	January 2017

Similar Records

Measurement Error in Atomic-Scale Scanning Transmission Electron Microscopy—Energy-Dispersive X-Ray Spectroscopy (STEM-EDS) Mapping of a Model Oxide Interface

Journal Article · Wed Apr 05 00:00:00 EDT 2017 · Microscopy and Microanalysis · OSTI ID:1361980

Fast Atomic-Scale Elemental Mapping of Crystalline Materials by STEM Energy-Dispersive X-Ray Spectroscopy Achieved with Thin Specimens [Fast Atomic-Scale Chemical Imaging of Crystalline Materials by STEM Energy-Dispersive X-ray Spectroscopy Achieved with Thin Specimens].

Journal Article · Wed Feb 22 19:00:00 EST 2017 · Microscopy and Microanalysis · OSTI ID:1356226

Performance and Image Analysis of the Aberration Corrected Hitachi HD-2700C Stem

Journal Article · Sat Feb 28 23:00:00 EST 2009 · Journal of Electron Microscopy · OSTI ID:1040244

Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Measurement Error in Atomic-Scale Scanning Transmission Electron Microscopy—Energy-Dispersive X-Ray Spectroscopy (STEM-EDS) Mapping of a Model Oxide Interface

Citation Formats

References (24)

Cited By (7)

Similar Records

Related Subjects