Imaging 3D chemistry at 1 nm resolution with fused multi-modal electron tomography

Jonathan Schwartz; Zichao Wendy Di; Yi Jiang; Jason Manassa; Jacob Pietryga; Yiwen Qian; Min Gee Cho; Jonathan L Rowell; Huihuo Zheng; Richard D Robinson; Junsi Gu; Alexey Kirilin; Steve Rozeveld; Peter Ercius; Jeffrey A Fessler; Ting Xu; Mary Scott; Robert Hovden

doi:10.1038/s41467-024-47558-0

Imaging 3D chemistry at 1 nm resolution with fused multi-modal electron tomography

Nat Commun. 2024 Apr 26;15(1):3555. doi: 10.1038/s41467-024-47558-0.

Authors

Jonathan Schwartz¹, Zichao Wendy Di², Yi Jiang³, Jason Manassa¹, Jacob Pietryga^{1

4}, Yiwen Qian⁵, Min Gee Cho^{5

6}, Jonathan L Rowell⁷, Huihuo Zheng⁸, Richard D Robinson^{9

10}, Junsi Gu¹¹, Alexey Kirilin¹², Steve Rozeveld¹³, Peter Ercius⁶, Jeffrey A Fessler¹⁴, Ting Xu^{5

15}, Mary Scott^{16

17}, Robert Hovden^{18

19}

Affiliations

¹ Department of Materials Science and Engineering, University of Michigan, Ann Arbor, MI, USA.
² Mathematics and Computer Science Division, Argonne National Laboratory, Lemont, IL, USA.
³ Advanced Photon Source Facility, Argonne National Laboratory, Lemont, IL, USA.
⁴ Department of Material Science and Engineering, Northwestern University, Evanston, IL, USA.
⁵ Department of Materials Science and Engineering, University of California at Berkeley, Berkeley, CA, USA.
⁶ National Center for Electron Microscopy, Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
⁷ Department of Chemistry and Chemical Biology, Cornell University, Ithaca, NY, USA.
⁸ Argonne Leadership Computing Facility, Argonne National Laboratory, Lemont, IL, USA.
⁹ Department of Material Science and Engineering, Cornell University, Ithaca, NY, USA.
¹⁰ Kavli Institute at Cornell for Nanoscale Science, Cornell University, Ithaca, NY, USA.
¹¹ Dow Chemical Co., Collegeville, PA, USA.
¹² Dow Chemical Co., Terneuzen, the Netherlands.
¹³ Dow Chemical Co., Midland, MI, USA.
¹⁴ Department of Electrical Engineering and Computer Science, University of Michigan, Ann Arbor, MI, USA.
¹⁵ Materials Science Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
¹⁶ Department of Materials Science and Engineering, University of California at Berkeley, Berkeley, CA, USA. mary.scott@berkeley.edu.
¹⁷ National Center for Electron Microscopy, Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA, USA. mary.scott@berkeley.edu.
¹⁸ Department of Materials Science and Engineering, University of Michigan, Ann Arbor, MI, USA. hovden@umich.edu.
¹⁹ Applied Physics Program, University of Michigan, Ann Arbor, MI, USA. hovden@umich.edu.

Abstract

Measuring the three-dimensional (3D) distribution of chemistry in nanoscale matter is a longstanding challenge for metrological science. The inelastic scattering events required for 3D chemical imaging are too rare, requiring high beam exposure that destroys the specimen before an experiment is completed. Even larger doses are required to achieve high resolution. Thus, chemical mapping in 3D has been unachievable except at lower resolution with the most radiation-hard materials. Here, high-resolution 3D chemical imaging is achieved near or below one-nanometer resolution in an Au-Fe₃O₄ metamaterial within an organic ligand matrix, Co₃O₄-Mn₃O₄ core-shell nanocrystals, and ZnS-Cu_0.64S_0.36 nanomaterial using fused multi-modal electron tomography. Multi-modal data fusion enables high-resolution chemical tomography often with 99% less dose by linking information encoded within both elastic (HAADF) and inelastic (EDX/EELS) signals. We thus demonstrate that sub-nanometer 3D resolution of chemistry is measurable for a broad class of geometrically and compositionally complex materials.