The projected electrostatic potential of a thick crystal is reconstructed at atomic resolution from experimental scanning transmission electron microscopy data recorded using a new generation fast-readout electron camera. This practical and deterministic inversion of the equations encapsulating multiple scattering that were written down by Bethe in 1928 removes the restriction of established methods to ultrathin (≲50  Å) samples. Instruments already coming on line can overcome the remaining resolution-limiting effects in this method due to finite probe-forming aperture size, spatial incoherence, and residual lens aberrations.

Four-dimensional scanning transmission electron microscopy (4D-STEM) is a technique where a full two-dimensional convergent beam electron diffraction (CBED) pattern is acquired at every STEM pixel scanned. Capturing the full diffraction pattern provides a rich dataset that potentially contains more information about the specimen than is contained in conventional imaging modes using conventional integrating detectors. Using 4D datasets in STEM from two specimens, monolayer MoS2 and bulk SrTiO3, we demonstrate multiple STEM imaging modes on a quantitative absolute intensity scale, including phase reconstruction of the transmission function via differential phase contrast imaging. Practical issues about sampling (i.e. number of detector pixels), signal-to-noise enhancement and data reduction of large 4D-STEM datasets are emphasized.