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Three-dimensional atomic imaging of crystalline nanoparticles

Abstract

Determining the three-dimensional (3D) arrangement of atoms in crystalline nanoparticles is important for nanometre-scale device engineering and also for applications involving nanoparticles, such as optoelectronics or catalysis. A nanoparticle’s physical and chemical properties are controlled by its exact 3D morphology, structure and composition1. Electron tomography enables the recovery of the shape of a nanoparticle from a series of projection images2,3,4. Although atomic-resolution electron microscopy has been feasible for nearly four decades, neither electron tomography nor any other experimental technique has yet demonstrated atomic resolution in three dimensions. Here we report the 3D reconstruction of a complex crystalline nanoparticle at atomic resolution. To achieve this, we combined aberration-corrected scanning transmission electron microscopy5,6,7, statistical parameter estimation theory8,9 and discrete tomography10,11. Unlike conventional electron tomography, only two images of the target—a silver nanoparticle embedded in an aluminium matrix—are sufficient for the reconstruction when combined with available knowledge about the particle’s crystallographic structure. Additional projections confirm the reliability of the result. The results we present help close the gap between the atomic resolution achievable in two-dimensional electron micrographs and the coarser resolution that has hitherto been obtained by conventional electron tomography.

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Figure 1: Quantification of HAADF STEM images.
Figure 2: Analysis of scattered intensities.
Figure 3: Three-dimensional reconstruction.
Figure 4: Comparison of experimental images with projected 3D reconstructions.

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Acknowledgements

Part of this work was performed at the National Center for Electron Microscopy (LBNL) which is supported by the Office of Science, Office of Basic Energy Sciences of the US Department of Energy under contract number DE-AC02-05CH11231. Financial support from the European Union for the Framework 6 programme under a contract for an Integrated Infrastructure Initiative (reference 026019 ESTEEM) is acknowledged.

Author information

Authors and Affiliations

Authors

Contributions

S.V.A. developed and applied a method of counting the number of atoms. K.J.B. reconstructed the nanoparticle in three dimensions. M.D.R. and R.E. prepared the sample and recorded the experimental images. G.V.T. advised on the methodology, the interpretation and on the paper. All the authors read and commented on the paper.

Corresponding author

Correspondence to Sandra Van Aert.

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Competing interests

The authors declare no competing financial interests.

Supplementary information

Supplementary Information

The file contains Supplementary Methods, Supplementary Table 1, Supplementary Figures 1-6 with legends and additional references. (PDF 572 kb)

Supplementary Movie 1

The movie shows the computed 3D reconstruction of a Ag nanocluster showing the 3D position of all 784 atoms. (MOV 16227 kb)

Supplementary Movie 2

The movie shows the computed 3D reconstruction in which the Ag nanocluster is tilted from the [101] zone-axis toward [100], [41 1], [21 1] , and back. (MOV 8517 kb)

Supplementary Movie 3

The movie shows the computed 3D reconstruction in which the Ag nanocluster is tilted from the [101] zone-axis toward [100], [41 1], [21 1], and back. This movie includes a confidence estimate for each atom position. The radius of the bright shell around the atoms represents the confidence that can be associated with a particular atom. Absence of the shell represents high confidence, while a large shell represents high uncertainty. (MOV 7998 kb)

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Van Aert, S., Batenburg, K., Rossell, M. et al. Three-dimensional atomic imaging of crystalline nanoparticles. Nature 470, 374–377 (2011). https://doi.org/10.1038/nature09741

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