We demonstrate spatially resolved diffractometry in which diffraction patterns are acquired at two-dimensional positions on a specimen using scanning transmission electron microscopy (STEM), resulting in four-dimensional data acquisition. A high spatial resolution of about 0.1 nm is achieved using a stabilized STEM instrument, a spherical aberration corrector and various post-acquisition data processings. We have found a few novel results in the radial and the azimuthal scattering angle dependences of atomic-column contrast in STEM images. Atomic columns are clearly observed in dark field images obtained using the excess Kikuchi band intensity even in small solid-angle detection. We also find that atomic-column contrasts in dark field images are shifted in the order of a few tens of picometers on changing the azimuthal scattering angle. This experimental result is approximately interpretable on the basis of the impact parameter in Rutherford scattering. Spatially resolved diffractometry provides fundamental knowledge related to various STEM techniques, such as annular dark field (ADF) and annular bright field (ABF) imaging, and it is expected to become an analytical platform for advanced STEM imaging.
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