Pushing the Dose Limit of Atomic-Resolution Imaging: A 4D-STEM case study of NaCl

Abstract

Beam-induced damage fundamentally limits the characterization of beam-sensitive materials by scanning transmission electron microscopy (STEM), since structural information must be recorded before the electron beam irreversibly modifies the specimen. Here, sodium chloride (NaCl) is employed as a model beam-sensitive ionic crystal to investigate beam-induced structural evolution and the low-dose regime in which useful structural information can be recovered prior to significant damage. Four-dimensional STEM (4D-STEM) datasets were acquired at 200 kV using a Timepix3 direct electron detector and reconstructed using real-time integrated centre of mass (riCoM) imaging. We first establish the characteristic damage behavior of NaCl under high electron doses. Across different dwell times and raster scan orientations, damage develops reproducibly into square-faceted voids whose boundaries align with the 100 crystallographic directions of the rock-salt lattice, indicating that the morphology is governed predominantly by the intrinsic crystallography rather than the scan geometry. We then investigate the low-dose imaging regime using dose-fractionated acquisitions. At 130 e-A-2 per frame, normalized cross-correlation with respect to the first frame quantitatively tracks progressive structural degradation and enables the onset of measurable damage to be identified as a function of accumulated dose. A subsequent acquisition at 32 e-A-2 per frame demonstrates that atomic-scale spatial information can still be recovered below this damage threshold. These results demonstrate how dose-efficient 4D-STEM acquisition combined with riCoM imaging can extend the accessible imaging regime of highly beam-sensitive ionic materials while preserving atomic-scale information.