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Virtual dark field and digital dark field imaging

Because a 4D-STEM dataset contains the entire diffraction pattern at every probe position, any STEM detector geometry can be applied after the experiment: integrate the intensity inside a chosen region of the diffraction pattern at each probe position, and the result is an image. This is virtual imaging, and it is usually the first, and often the most informative, analysis applied to any 4D-STEM dataset. Virtual bright field and dark field reconstruction in this sense was popularized by Rauch and co-workers alongside scanning precession diffraction and ACOM VILADOT et al. (2013), Rauch & Véron (2014), and generalized to arbitrarily shaped virtual apertures by Gammer et al. Gammer et al. (2015).

Virtual bright field and dark field

A circular mask over the central beam gives a virtual bright field (BF) image; an annulus outside it gives a virtual annular dark field (ADF). The two are complementary: electrons scattered out of the BF disk land in the DF detector, so regions that darken in BF brighten in DF. Unlike physical detectors, virtual detectors are free: you can try any inner/outer radius, any shape, any position, and iterate until the contrast isolates the feature you care about Paterson et al. (2020):

Virtual detector geometries applied to a diffraction pattern: a single aperture, an annular aperture, and an array of apertures over the diffracted spots

Virtual detectors are defined in software after the experiment: a single aperture over one reflection, an annulus, or an aperture array matched to a whole family of diffracted spots.

Digital dark field

Classical dark field TEM tilts the beam (or shifts the objective aperture) so one chosen Bragg reflection forms the image:

Ray diagram of dark field imaging in conventional TEM using an objective aperture in the back focal plane

Conventional dark field TEM: an objective aperture in the back focal plane selects a single diffracted beam to form the image: one reflection, one exposure, one tilt condition at a time.

The 4D-STEM equivalent, digital dark field (DDF) MacLaren et al. (2024), places a virtual aperture over one (or several) specific Bragg reflections and maps where in real space that reflection is excited. Every reflection in the dataset is available simultaneously, from a single scan:

Flowchart of the digital dark field workflow, from probe template and peak finding through single apertures, aperture arrays, or points-list reduction to virtual dark field images

The DDF workflow: after peak finding and g-vector identification, images can be formed from a single virtual aperture, from a mask built on a whole array of aperture positions, or by reducing the detected points list directly against the aperture array.

This is enormously powerful for microstructure:

Digital dark field maps of a perovskite film formed from different superlattice and higher-order Laue zone reflections, each highlighting a different ordered region

Digital dark field in action on a perovskite thin film: virtual apertures on different superlattice and higher-order Laue zone reflections (right) map chemically and structurally distinct ordered regions through the film (left), all from one 4D-STEM scan.

References
  1. VILADOT, D., VÉRON, M., GEMMI, M., PEIRÓ, F., PORTILLO, J., ESTRADÉ, S., MENDOZA, J., LLORCA‐ISERN, N., & NICOLOPOULOS, S. (2013). Orientation and phase mapping in the transmission electron microscope using precession‐assisted diffraction spot recognition: state‐of‐the‐art results. Journal of Microscopy, 252(1), 23–34. 10.1111/jmi.12065
  2. Rauch, E. F., & Véron, M. (2014). Automated crystal orientation and phase mapping in TEM. Materials Characterization, 98, 1–9. 10.1016/j.matchar.2014.08.010
  3. Gammer, C., Burak Ozdol, V., Liebscher, C. H., & Minor, A. M. (2015). Diffraction contrast imaging using virtual apertures. Ultramicroscopy, 155, 1–10. 10.1016/j.ultramic.2015.03.015
  4. Paterson, G. W., Webster, R. W. H., Ross, A., Paton, K. A., Macgregor, T. A., McGrouther, D., MacLaren, I., & Nord, M. (2020). Fast Pixelated Detectors in Scanning Transmission Electron Microscopy. Part II: Post-Acquisition Data Processing, Visualization, and Structural Characterization. Microscopy and Microanalysis, 26(5), 944–963. 10.1017/s1431927620024307
  5. MacLaren, I., Fraser, A. T., Lipsett, M. R., & Ophus, C. (2024). Digital Dark Field—Higher Contrast and Greater Specificity Dark Field Imaging Using a 4DSTEM Approach. Microscopy and Microanalysis, 31(1). 10.1093/mam/ozae104
  6. MacLaren, I., Frutos-Myro, E., McGrouther, D., McFadzean, S., Weiss, J. K., Cosart, D., Portillo, J., Robins, A., Nicolopoulos, S., Nebot del Busto, E., & Skogeby, R. (2020). A Comparison of a Direct Electron Detector and a High-Speed Video Camera for a Scanning Precession Electron Diffraction Phase and Orientation Mapping. Microscopy and Microanalysis, 26(6), 1110–1116. 10.1017/s1431927620024411