Electron energy loss spectroscopy database synthesis and automation of core-loss edge recognition by deep-learning neural networks

Kong, Lingli; Ji, Zhengran; Xin, Huolin L.

doi:10.1038/s41598-022-25870-3

Title: Electron energy loss spectroscopy database synthesis and automation of core-loss edge recognition by deep-learning neural networks

Journal Article · 22 December 2022 · Scientific Reports

DOI: https://doi.org/10.1038/s41598-022-25870-3 · OSTI ID:1906537

Kong, Lingli; Ji, Zhengran; Xin, Huolin L.

Abstract The ionization edges encoded in the electron energy loss spectroscopy (EELS) spectra enable advanced material analysis including composition analyses and elemental quantifications. The development of the parallel EELS instrument and fast, sensitive detectors have greatly improved the acquisition speed of EELS spectra. However, the traditional way of core-loss edge recognition is experience based and human labor dependent, which limits the processing speed. So far, the low signal–noise ratio and the low jump ratio of the core-loss edges on the raw EELS spectra have been challenging for the automation of edge recognition. In this work, a convolutional-bidirectional long short-term memory neural network (CNN-BiLSTM) is proposed to automate the detection and elemental identification of core-loss edges from raw spectra. An EELS spectral database is synthesized by using our forward model to assist in the training and validation of the neural network. To make the synthesized spectra resemble the real spectra, we collected a large library of experimentally acquired EELS core edges. In synthesize the training library, the edges are modeled by fitting the multi-Gaussian model to the real edges from experiments, and the noise and instrumental imperfectness are simulated and added. The well-trained CNN-BiLSTM network is tested against both the simulated spectra and real spectra collected from experiments. The high accuracy of the network, 94.9%, proves that, without complicated preprocessing of the raw spectra, the proposed CNN-BiLSTM network achieves the automation of core-loss edge recognition for EELS spectra with high accuracy.

View Journal Article

Cite

Export

Save

Research Organization:: Univ. of California, Irvine, CA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: SC0021204

OSTI ID:: 1906537

Journal Information:: Scientific Reports, Journal Name: Scientific Reports Journal Issue: 1 Vol. 12; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

References (66)

Electrochemically Driven Giant Resistive Switching in Perovskite Nickelates Heterostructures Wang, Le; Zhang, Qinghua; Chang, Lei Advanced Electronic Materials, Vol. 3, Issue 10 https://doi.org/10.1002/aelm.201700321	journal	August 2017
Machine learning tools formineral recognition and classification from Raman spectroscopy: Tools for mineral recognition and classification from RS Carey, C.; Boucher, T.; Mahadevan, S. Journal of Raman Spectroscopy, Vol. 46, Issue 10 https://doi.org/10.1002/jrs.4757	journal	August 2015
Electron Energy Loss Spectroscopy (EELS) Li, Wanfeng; Ni, Chaoying Encyclopedia of Tribology https://doi.org/10.1007/978-0-387-92897-5_1223	book	January 2013
Electron Energy Loss Spectroscopy for Single Atom Catalysis Gao, Zirui; Li, Aowen; Ma, Ding Topics in Catalysis https://doi.org/10.1007/s11244-022-01577-7	journal	February 2022
Nonstoichiometric Titanium Oxides via Pulsed Laser Ablation in Water Huang, Chang-Ning; Bow, Jong-Shing; Zheng, Yuyuan Nanoscale Research Letters, Vol. 5, Issue 6 https://doi.org/10.1007/s11671-010-9591-4	journal	April 2010
Electric field-triggered metal-insulator transition resistive switching of bilayered multiphasic VOx Won, Seokjae; Lee, Sang Yeon; Hwang, Jungyeon Electronic Materials Letters, Vol. 14, Issue 1 https://doi.org/10.1007/s13391-017-7134-1	journal	October 2017
Extracting information from sequences of spatially resolved EELS spectra using multivariate statistical analysis Bonnet, N.; Brun, N.; Colliex, C. Ultramicroscopy, Vol. 77, Issue 3-4 https://doi.org/10.1016/S0304-3991(99)00042-X	journal	July 1999
Local chemical states and microstructure of photoluminescent porous silicon studied by means of EELS and TEM Song, M.; Fukuda, Y.; Furuya, K. Micron, Vol. 31, Issue 4 https://doi.org/10.1016/S0968-4328(99)00120-1	journal	August 2000
Microstructural characterization of boron-rich boron carbide Xie, Kelvin Y.; Domnich, Vladislav; Farbaniec, Lukasz Acta Materialia, Vol. 136 https://doi.org/10.1016/j.actamat.2017.06.063	journal	September 2017
Electron-energy loss spectroscopy and Raman studies of nanosized chromium carbide synthesized during carbothermal reduction process from precursor Cr(CO)6 Lin, Hao-Tung; Nayak, Pramoda K.; Wang, Sheng-Chang Journal of the European Ceramic Society, Vol. 31, Issue 14 https://doi.org/10.1016/j.jeurceramsoc.2010.12.005	journal	November 2011
Characterization of two phase distribution in electrochemically-lithiated spinel Li4Ti5O12 secondary particles by electron energy-loss spectroscopy Kitta, Mitsunori; Akita, Tomoki; Tanaka, Shingo Journal of Power Sources, Vol. 237 https://doi.org/10.1016/j.jpowsour.2013.03.022	journal	September 2013
Application of EELS in Materials Science Keast, V. J. Materials Characterization, Vol. 73 https://doi.org/10.1016/j.matchar.2012.07.013	journal	November 2012
A STEM/EELS method for mapping iron valence ratios in oxide minerals Cavé, Lisa; Al, Tom; Loomer, Diana Micron, Vol. 37, Issue 4 https://doi.org/10.1016/j.micron.2005.10.006	journal	June 2006
High resolution EELS of Cu–V oxides: Application to batteries materials Laffont, L.; Wu, M. Y.; Chevallier, F. Micron, Vol. 37, Issue 5 https://doi.org/10.1016/j.micron.2005.11.007	journal	July 2006
Effect of strontium ranelate on bone mineral: Analysis of nanoscale compositional changes Rossi, André L.; Moldovan, Simona; Querido, William Micron, Vol. 56 https://doi.org/10.1016/j.micron.2013.09.008	journal	January 2014
Model based quantification of EELS spectra Verbeeck, J.; Van Aert, S. Ultramicroscopy, Vol. 101, Issue 2-4 https://doi.org/10.1016/j.ultramic.2004.06.004	journal	November 2004
Independent component analysis: A new possibility for analysing series of electron energy loss spectra Bonnet, Noël; Nuzillard, Danielle Ultramicroscopy, Vol. 102, Issue 4 https://doi.org/10.1016/j.ultramic.2004.11.003	journal	March 2005
Mapping titanium and tin oxide phases using EELS: An application of independent component analysis de la Peña, F.; Berger, M. -H.; Hochepied, J. -F. Ultramicroscopy, Vol. 111, Issue 2 https://doi.org/10.1016/j.ultramic.2010.10.001	journal	January 2011
Oxidation state and chemical shift investigation in transition metal oxides by EELS Tan, Haiyan; Verbeeck, Jo; Abakumov, Artem Ultramicroscopy, Vol. 116 https://doi.org/10.1016/j.ultramic.2012.03.002	journal	May 2012
Strong excitonic interactions in the oxygen K-edge of perovskite oxides Tomita, Kota; Miyata, Tomohiro; Olovsson, Weine Ultramicroscopy, Vol. 178 https://doi.org/10.1016/j.ultramic.2016.04.006	journal	July 2017
Accurate EELS background subtraction – an adaptable method in MATLAB Fung, Kayleigh L. Y.; Fay, Michael W.; Collins, Sean M. Ultramicroscopy, Vol. 217 https://doi.org/10.1016/j.ultramic.2020.113052	journal	October 2020
Nickel Impurities in the Solid-Electrolyte Interphase of Lithium-Metal Anodes Revealed by Cryogenic Electron Microscopy Vilá, Rafael A.; Huang, William; Cui, Yi Cell Reports Physical Science, Vol. 1, Issue 9 https://doi.org/10.1016/j.xcrp.2020.100188	journal	September 2020
Electron Energy Loss Spectroscopy (EELS) of Iron Fischer–Tropsch Catalysts Jin, Yaming; Xu, Huifang; Datye, Abhaya K. Microscopy and Microanalysis, Vol. 12, Issue 2 https://doi.org/10.1017/S1431927606060144	journal	March 2006
The Real Carbon K-Edge Alexander, Dtl; Anderson, Jr; Forró, L. Microscopy and Microanalysis, Vol. 14, Issue S2 https://doi.org/10.1017/S1431927608086509	journal	August 2008
Data Processing for Atomic Resolution Electron Energy Loss Spectroscopy Cueva, Paul; Hovden, Robert; Mundy, Julia A. Microscopy and Microanalysis, Vol. 18, Issue 4 https://doi.org/10.1017/S1431927612000244	journal	June 2012
In Situ Observation of Electron Beam-Induced Phase Transformation of CaCO₃ to CaO via ELNES at Low Electron Beam Energies Golla-Schindler, Ute; Benner, Gerd; Orchowski, Alexander Microscopy and Microanalysis, Vol. 20, Issue 3 https://doi.org/10.1017/S1431927614000464	journal	April 2014
A Complete Overhaul of the Electron Energy-Loss Spectroscopy and X-Ray Absorption Spectroscopy Database: eelsdb.eu Ewels, Philip; Sikora, Thierry; Serin, Virginie Microscopy and Microanalysis, Vol. 22, Issue 3 https://doi.org/10.1017/S1431927616000179	journal	February 2016
Carrier Mobility Enhancement of Tensile Strained Si and SiGe Nanowires via Surface Defect Engineering Ma, J. W.; Lee, W. J.; Bae, J. M. Nano Letters, Vol. 15, Issue 11 https://doi.org/10.1021/acs.nanolett.5b01634	journal	October 2015
Multiple Scattering Calculations of Bonding and X-ray Absorption Spectroscopy of Manganese Oxides Gilbert, B.; Frazer, B. H.; Belz, A. The Journal of Physical Chemistry A, Vol. 107, Issue 16 https://doi.org/10.1021/jp021493s	journal	April 2003
Structure and bonding at the atomic scale by scanning transmission electron microscopy Muller, David A. Nature Materials, Vol. 8, Issue 4 https://doi.org/10.1038/nmat2380	journal	April 2009
Near-edge X-ray absorption fine-structure microscopy of organic and magnetic materials Ade, Harald; Stoll, Herman Nature Materials, Vol. 8, Issue 4 https://doi.org/10.1038/nmat2399	journal	April 2009
Three dimensional band-filling control of complex oxides triggered by interfacial electron transfer Meng, Meng; Sun, Yuanwei; Li, Yuehui Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-22790-0	journal	April 2021
The effects of oxygen in spinel oxide Li1+xTi2−xO4−δ thin films Jia, Yanli; He, Ge; Hu, Wei Scientific Reports, Vol. 8, Issue 1 https://doi.org/10.1038/s41598-018-22393-8	journal	March 2018
Towards calibration-invariant spectroscopy using deep learning Chatzidakis, M.; Botton, G. A. Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-019-38482-1	journal	February 2019
Combined study of the ground and excited states in the transformation of nanodiamonds into carbon onions by electron energy-loss spectroscopy Feng, Zhenbao; Lin, Yangming; Tian, Cunwei Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-019-40529-2	journal	March 2019
Visualization of chemical bonding in a silica-filled rubber nanocomposite using STEM-EELS Sato, Yohei K.; Kuwauchi, Yasufumi; Miyoshi, Wakana Scientific Reports, Vol. 10, Issue 1 https://doi.org/10.1038/s41598-020-78393-0	journal	December 2020
RapidEELS: machine learning for denoising and classification in rapid acquisition electron energy loss spectroscopy Pate, Cassandra M.; Hart, James L.; Taheri, Mitra L. Scientific Reports, Vol. 11, Issue 1 https://doi.org/10.1038/s41598-021-97668-8	journal	September 2021
In situ TEM Observation of Resistance Switching in Titanate Based Device Yang, Yang; Lü, Weiming; Yao, Yuan Scientific Reports, Vol. 4, Issue 1 https://doi.org/10.1038/srep03890	journal	January 2014
Enhanced Thermoelectric Performance in Cu-Intercalated BiTeI by Compensation Weakening Induced Mobility Improvement Wu, Lihua; Yang, Jiong; Chi, Miaofang Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep14319	journal	September 2015
Novel hybrid nanocomposites of polyhedral Cu₂O nanoparticles–CuO nanowires with enhanced photoactivity Wang, Chao; Wang, Yiqian; Liu, Xuehua Phys. Chem. Chem. Phys., Vol. 16, Issue 33 https://doi.org/10.1039/C4CP01696C	journal	January 2014
Profiling the nanoscale gradient in stoichiometric layered cathode particles for lithium-ion batteries Lin, Feng; Nordlund, Dennis; Markus, Isaac M. Energy & Environmental Science, Vol. 7, Issue 9 https://doi.org/10.1039/C4EE01400F	journal	January 2014
Influence of synthesis conditions on the surface passivation and electrochemical behavior of layered cathode materials Lin, Feng; Nordlund, Dennis; Pan, Taijun J. Mater. Chem. A, Vol. 2, Issue 46 https://doi.org/10.1039/C4TA04497E	journal	January 2014
Spatially resolved surface valence gradient and structural transformation of lithium transition metal oxides in lithium-ion batteries Liu, Hanshuo; Bugnet, Matthieu; Tessaro, Matteo Z. Physical Chemistry Chemical Physics, Vol. 18, Issue 42 https://doi.org/10.1039/C6CP05262B	journal	January 2016
Systematic analysis of electron energy-loss near-edge structures in Li-ion battery materials Saitoh, Motofumi; Gao, Xiang; Ogawa, Takafumi Physical Chemistry Chemical Physics, Vol. 20, Issue 38 https://doi.org/10.1039/C8CP03390K	journal	January 2018
Probing the electrode/electrolyte interface in the lithium excess layered oxide Li1.2Ni0.2Mn0.6O2 Carroll, Kyler J.; Qian, Danna; Fell, Chris Physical Chemistry Chemical Physics, Vol. 15, Issue 26 https://doi.org/10.1039/c3cp51927a	journal	January 2013
Characterisation of Co@Fe3O4 core@shell nanoparticles using advanced electron microscopy Knappett, Benjamin R.; Abdulkin, Pavel; Ringe, Emilie Nanoscale, Vol. 5, Issue 13 https://doi.org/10.1039/c3nr33789h	journal	January 2013
Structural phase transformation and Fe valence evolution in FeOxF2−x/C nanocomposite electrodes during lithiation and de-lithiation processes Sina, M.; Nam, K. -W.; Su, D. Journal of Materials Chemistry A, Vol. 1, Issue 38 https://doi.org/10.1039/c3ta12109g	journal	January 2013
Characterization of carbon nitride thin films prepared by dual ion beam sputtering Fernández, A.; Prieto, P.; Quirós, C. Applied Physics Letters, Vol. 69, Issue 6 https://doi.org/10.1063/1.117884	journal	August 1996
Site determination and magnetism of Mn doping in protein encapsulated iron oxide nanoparticles Pool, V.; Klem, M.; Jolley, C. Journal of Applied Physics, Vol. 107, Issue 9 https://doi.org/10.1063/1.3359431	journal	May 2010
Atomic and electronic structures of the SrVO ₃ -LaAlO ₃ interface Chi, Miaofang; Mizoguchi, Teruyasu; Martin, Lane W. Journal of Applied Physics, Vol. 110, Issue 4 https://doi.org/10.1063/1.3601870	journal	August 2011
Magnetic and electronic properties of the interface between half metallic Fe ₃ O ₄ and semiconducting ZnO Brück, S.; Paul, M.; Tian, H. Applied Physics Letters, Vol. 100, Issue 8 https://doi.org/10.1063/1.3687731	journal	February 2012
X-ray absorption of Si–C–N thin films: A comparison between crystalline and amorphous phases Chang, Y. K.; Hsieh, H. H.; Pong, W. F. Journal of Applied Physics, Vol. 86, Issue 10 https://doi.org/10.1063/1.371568	journal	November 1999
On the local electronic and atomic structure of Ce_1−xPr_xO_2−δ epitaxial films on Si Niu, Gang; Schubert, Markus Andreas; d'Acapito, Francesco Journal of Applied Physics, Vol. 116, Issue 12 https://doi.org/10.1063/1.4896590	journal	September 2014
Structure versus properties inα-Fe₂O₃nanowires and nanoblades Wang, Chao; Wang, Yiqian; Liu, Xuehua Nanotechnology, Vol. 27, Issue 3 https://doi.org/10.1088/0957-4484/27/3/035702	journal	December 2015
Transmission electron microscopy/electron energy loss spectroscopy measurements andab initiocalculation of local magnetic moments at nickel grain boundaries Hirayama, Kyosuke; Ii, Seiichiro; Tsurekawa, Sadahiro Science and Technology of Advanced Materials, Vol. 15, Issue 1 https://doi.org/10.1088/1468-6996/15/1/015005	journal	February 2014
High throughput production of nanocomposite SiO_x powders by plasma spray physical vapor deposition for negative electrode of lithium ion batteries Homma, Keiichiro; Kambara, Makoto; Yoshida, Toyonobu Science and Technology of Advanced Materials, Vol. 15, Issue 2 https://doi.org/10.1088/1468-6996/15/2/025006	journal	April 2014
Electronic structure of titania-based nanotubes investigated by EELS spectroscopy Gloter, Alexandre; Ewels, Christopher; Umek, Polona Physical Review B, Vol. 80, Issue 3 https://doi.org/10.1103/PhysRevB.80.035413	journal	July 2009
Oxygen vacancy dipoles in strained epitaxial BaTiO3 films Tyunina, M.; Peräntie, J.; Kocourek, T. Physical Review Research, Vol. 2, Issue 2 https://doi.org/10.1103/PhysRevResearch.2.023056	journal	April 2020
Prebiotic carbon in clays from Orgueil and Ivuna (CI), and Tagish Lake (C2 ungrouped) meteorites Garvie, Laurence A. J.; Buseck, Peter R. Meteoritics & Planetary Science, Vol. 42, Issue 12 https://doi.org/10.1111/j.1945-5100.2007.tb01011.x	journal	December 2007
Analytical Transmission Electron Microscopy Sigle, Wilfried Annual Review of Materials Research, Vol. 35, Issue 1 https://doi.org/10.1146/annurev.matsci.35.102303.091623	journal	August 2005
Reaction Mechanism of “SiO”-Carbon Composite-Negative Electrode for High-Capacity Lithium-Ion Batteries Yamada, Masayuki; Inaba, Akira; Ueda, Atsushi Journal of The Electrochemical Society, Vol. 159, Issue 10 https://doi.org/10.1149/2.018210jes	journal	January 2012
Improving the Wettability of Thin-Film Rotating Disk Electrodes for Reliable Activity Evaluation of Oxygen Electrocatalysts by Triggering Oxygen Reduction at the Catalyst-Electrolyte-Bubble Triple Phase Boundaries Wang, Ruozheng; Jiang, Wulv; Xia, Dongsheng Journal of The Electrochemical Society, Vol. 165, Issue 7 https://doi.org/10.1149/2.0371807jes	journal	January 2018
Nanoscale chemical and structural study of Co-based FEBID structures by STEM-EELS and HRTEM Córdoba, Rosa; Fernández-Pacheco, Rodrigo; Fernández-Pacheco, Amalio Nanoscale Research Letters, Vol. 6, Issue 1 https://doi.org/10.1186/1556-276X-6-592	journal	January 2011
Boosting optical nonreciprocity: surface reconstruction in iron garnets Dash, Sushree S.; Mukherjee, Pinaki; Haskel, Daniel Optica, Vol. 7, Issue 9 https://doi.org/10.1364/OPTICA.398732	journal	January 2020
Parallel electron energy-loss spectroscopy (PEELS) study of B in minerals; the electron energy-loss near-edge structure (ELNES) of the B K edge Garvie, Laurence A. J.; Craven, Alan J.; Brydson, Rik American Mineralogist, Vol. 80, Issue 11-12 https://doi.org/10.2138/am-1995-11-1204	journal	December 1995
Kishonite, VH2, and Oreillyite, Cr2N, Two New Minerals from the Corundum Xenocrysts of Mt Carmel, Northern Israel Bindi, Luca; Cámara, Fernando; Gain, Sarah E. M. Minerals, Vol. 10, Issue 12 https://doi.org/10.3390/min10121118	journal	December 2020

Similar Records

MnEdgeNet for accurate decomposition of mixed oxidation states for Mn XAS and EELS L2,3 edges without reference and calibration

Journal Article · 2023 · Scientific Reports · OSTI ID:2421806

Ji, Zhengran; Hu, Mike; Xin, Huolin L.

Deep Learning for Automated Detection and Identification of Migrating American Eel Anguilla rostrata from Imaging Sonar Data

Journal Article · 2021 · Remote Sensing · OSTI ID:1808592

Zang, Xiaoqin; Yin, Tianzhixi; Hou, Zhangshuan; +3 more

A comparison of machine learning methods for automated gamma-ray spectroscopy

Journal Article · 2018 · Nuclear Instruments and Methods in Physics Research. Section A, Accelerators, Spectrometers, Detectors and Associated Equipment · OSTI ID:1524430

Kamuda, Mark; Zhao, Jifu; Huff, Kathryn

Related Subjects

36 MATERIALS SCIENCE
Science & Technology - Other Topics

Title: Electron energy loss spectroscopy database synthesis and automation of core-loss edge recognition by deep-learning neural networks

Citation Formats

References (66)

Similar Records

Related Subjects