Dynamical diffraction of high-energy electrons investigated by focal series momentum-resolved scanning transmission electron microscopy at atomic resolution.

We report a study of scattering dynamics in crystals employing momentum-resolved scanning transmission electron microscopy under varying illumination conditions. As we perform successive changes of the probe focus, multiple real-space signals are obtained in dependence of the shape of the incident electron wave. With support from extensive simulations, each signal is shown to be characterised by an optimum focus for which the contrast is maximum and which differs among different signals. For instance, a systematic focus mismatch is found between images formed by high-angle scattering, being sensitive to thickness and chemical composition, and the first moment in diffraction space, being sensitive to electric fields. It follows that a single recording at one specific probe focus is usually insufficient to characterise materials comprehensively. Most importantly, we demonstrate in experiment and simulation that the second moment µ20+µ02=〈p2〉 of the diffracted intensity exhibits a contrast maximum when the electron probe is focused at the top and bottom faces of the specimen, making the presented concept attractive for measuring local topography. Given the versatility of 〈p2〉, we furthermore present a detailed study of its large-angle convergence both analytically using the Mott scattering approach, and by dynamical simulations using the multislice algorithm including thermal diffuse scattering. Both approaches are in very good agreement and yield logarithmic divergence with increasing scattering angle.