A schematic diagram of the experiment. The sample, a gold nanostructure supported on a silicon nitride membrane, was rotated about the y axis by an angle θ to obtain diffraction patterns at different orientations with respect to the optical axis z. A first rotation series about the y axis was followed by an in-plane rotation of the sample about z (angle χ) and a subsequent second rotation series about y. The beam attenuation and illumination time were adjusted so that each data frame contains only about 50 scattered photons. An example of a single diffraction pattern is shown in the inset on the upper left-hand side (see also animation in the supporting information). The area of a single pixel in comparison with the field-of-view area has been enlarged for visualization.