journal article·2024-03-12Open access

Robust Machine Learning Inference from X-ray Absorption Near Edge Spectra through Featurization

Yiming Chen, Chi Chen, Inhui Hwang, Michael J. Davis, Wanli Yang, Chengjun Sun, Gi-Hyeok Lee, Dylan McReynolds, Daniel Allan, Juan Marulanda Arias, Shyue Ping Ong, Maria K. Y. Chan

Chemistry of Materials· Volume 36· Issue 5

Abstract

X-ray absorption spectroscopy (XAS) is a commonly employed technique for characterizing functional materials. In particular, X-ray absorption near edge spectra (XANES) encode local coordination and electronic information, and machine learning approaches to extract this information are of significant interest. To date, most ML approaches for XANES have primarily focused on using the raw spectral intensities as input, overlooking the potential benefits of incorporating spectral transformations and dimensionality reduction techniques into ML predictions. In this work, we focused on systematically comparing the impact of different featurization methods on the performance of ML models for XAS analysis. We evaluated the classification and regression capabilities of these models on computed data sets and validated their performance on previously unseen experimental data sets. Our analysis revealed an intriguing discovery: the cumulative distribution function feature achieves both high prediction accuracy and exceptional transferability. This remarkably robust performance can be attributed to its tolerance to horizontal shifts in the spectra, which is crucial when validating models using experimental data. While this work exclusively focuses on XANES analysis, we anticipate that the methodology presented here will hold promise as a versatile asset to the broader spectroscopy community.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Machine Learning in Materials Science · X-ray Spectroscopy and Fluorescence Analysis · Advanced X-ray and CT Imaging

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of NanoEngineering, University of California San Diego, 9500 Gilman Dr, La Jolla, California 92093, United States

Center for Nanoscale Materials, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United States

Advanced Photon Source, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United States

Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United States

Advanced Light Source, Lawrence Berkeley National Laboratory, 6 Cyclotron Rd, Berkeley, California 94720, United States

National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, New York 11973, United States

Funding

Basic Energy Sciences · Advanced Light Source · Office of Advanced Cyberinfrastructure

References (60)

Show source-provided references
1. 10.1107/S090904951000623010.1107/S0909049510006230 ↗
2. 10.1039/b104782p10.1039/b104782p ↗
3. 10.1021/acs.est.8b0639110.1021/acs.est.8b06391 ↗
4. 10.1038/s41524-020-00376-610.1038/s41524-020-00376-6 ↗
5. 10.1038/s41524-022-00734-610.1038/s41524-022-00734-6 ↗
6. 10.2138/rmg.2014.78.210.2138/rmg.2014.78.2 ↗
7. 10.1103/RevModPhys.72.62110.1103/RevModPhys.72.621 ↗
8. 10.1016/j.ccr.2004.03.01810.1016/j.ccr.2004.03.018 ↗
9. 10.1103/PhysRevB.82.20510410.1103/PhysRevB.82.205104 ↗
10. 10.1038/sdata.2018.15110.1038/sdata.2018.151 ↗
11. 10.1038/s41597-021-00936-510.1038/s41597-021-00936-5 ↗
12. 10.1016/j.cattod.2018.10.07110.1016/j.cattod.2018.10.071 ↗
13. 10.1557/s43577-022-00446-810.1557/s43577-022-00446-8 ↗
14. 10.1039/C9ME00043G10.1039/C9ME00043G ↗
15. 10.1103/physrevb.103.04514010.1103/physrevb.103.045140 ↗
16. Li, L.; Lu, M.; Chan, M. K. Y. A Deep Learning Model for Atomic Structures Prediction Using X-ray Absorption Spectroscopic Data. 2019, arXiv:1905.03928, (accessed Dec 13, 2019).
17. 10.1103/PhysRevMaterials.3.03360410.1103/PhysRevMaterials.3.033604 ↗
18. 10.1016/j.patter.2020.10001310.1016/j.patter.2020.100013 ↗
19. 10.1103/PhysRevLett.124.15640110.1103/PhysRevLett.124.156401 ↗
20. 10.1039/D3DD00101F10.1039/D3DD00101F ↗
21. 10.1021/acs.chemmater.1c0427910.1021/acs.chemmater.1c04279 ↗
22. 10.1002/advs.20200421410.1002/advs.202004214 ↗
23. 10.1039/D1CP02903G10.1039/D1CP02903G ↗
24. 10.1021/acs.jpclett.0c0379210.1021/acs.jpclett.0c03792 ↗
25. 10.1038/s41467-020-15355-010.1038/s41467-020-15355-0 ↗
26. 10.1021/acs.chemmater.9b0406610.1021/acs.chemmater.9b04066 ↗
27. Pedregosa F. · J. Mach. Learn. Res. · 2011 · 12 · 2825
28. 10.1107/S090904950703190110.1107/S0909049507031901 ↗
29. 10.2138/am-2003-042310.2138/am-2003-0423 ↗
30. 10.1016/j.cpc.2008.12.02010.1016/j.cpc.2008.12.020 ↗
31. 10.1037/h007132510.1037/h0071325 ↗
32. 10.1080/1478644010946272010.1080/14786440109462720 ↗
33. 10.1063/5.004911110.1063/5.0049111 ↗
34. 10.1126/science.290.5500.231910.1126/science.290.5500.2319 ↗
35. Abadi, M.; TensorFlow: A system for large-scale machine learning. 2016, arXiv:1605.08695, (accessed May 23, 2022).
36. 10.1021/acsmaterialslett.9b0009910.1021/acsmaterialslett.9b00099 ↗
37. 10.1021/acs.jpclett.7b0080910.1021/acs.jpclett.7b00809 ↗
38. 10.1002/adfm.20180795110.1002/adfm.201807951 ↗
39. 10.1107/S090904950501271910.1107/S0909049505012719 ↗
40. 10.1039/C4RA17235C10.1039/C4RA17235C ↗
41. 10.1038/s41467-022-28793-910.1038/s41467-022-28793-9 ↗
42. Rohatgi, A. Webplotdigitizer: Version 4.6; Webplotdigitizer, 2022.
43. 10.1103/PhysRevB.54.1116910.1103/PhysRevB.54.11169 ↗
44. 10.1103/PhysRevB.50.1795310.1103/PhysRevB.50.17953 ↗
45. 10.1103/PhysRevLett.115.03640210.1103/PhysRevLett.115.036402 ↗
46. 10.1038/s41524-020-00430-310.1038/s41524-020-00430-3 ↗
47. 10.1021/cm200753g10.1021/cm200753g ↗
48. 10.1021/acs.chemmater.7b0409610.1021/acs.chemmater.7b04096 ↗
49. 10.1021/acs.chemmater.0c0158210.1021/acs.chemmater.0c01582 ↗
50. 10.1063/1.481232310.1063/1.4812323 ↗
51. 10.1016/j.commatsci.2012.10.02810.1016/j.commatsci.2012.10.028 ↗
52. 10.1103/PhysRevB.98.23520510.1103/PhysRevB.98.235205 ↗
53. 10.1039/b926434e10.1039/b926434e ↗
54. 10.1088/0953-8984/21/34/34550110.1088/0953-8984/21/34/345501 ↗
55. 10.1103/PhysRevB.83.11510610.1103/PhysRevB.83.115106 ↗
56. 10.1016/j.elspec.2014.07.00510.1016/j.elspec.2014.07.005 ↗
57. 10.1021/acs.jpclett.2c0062810.1021/acs.jpclett.2c00628 ↗
58. 10.1063/5.006968110.1063/5.0069681 ↗
59. 10.1063/5.008738510.1063/5.0087385 ↗
60. 10.1063/5.016646910.1063/5.0166469 ↗