To date, high-resolution (< 1 nm) imaging of extended objects in three-dimensions (3D) has not been possible. A restriction known as the Crowther criterion forces a tradeoff between object size and resolution for 3D reconstructions by tomography. Further, the sub-Angstrom resolution of aberrationcorrected electron microscopes is accompanied by a greatly diminished depth of field, causing regions of larger specimens (> 6 nm) to appear blurred or missing. Here we demonstrate a three-dimensional imaging method that overcomes both these limits by combining through-focal depth sectioning and traditional tilt-series tomography to reconstruct extended objects, with high-resolution, in all three dimensions. The large convergence angle in aberration corrected instruments now becomes a benefit and not a hindrance to higher quality reconstructions. A through-focal reconstruction over a 390 nm 3D carbon support containing over one hundred dealloyed and nanoporous PtCu catalyst particles revealed with sub-nanometer detail the extensive and connected interior pore structure that is created by the dealloying instability.
IntroductionWith electron beams smaller than the bond length of hydrogen, aberration-corrected scanning transmission electron microscopes (STEM) can image materials with resolutions below the shortest bond lengths in nature 1 . However, these atomic resolution images are only 2D projections of a specimen. In order to determine the full 3D structure, one must acquire a series of STEM images over a range of specimen tilts 2,3 . Unfortunately, the resolution of a 3D STEM tomogram is degraded by missing information that is a consequence of the restricted specimen tilt range and finite tilt increments. While reconstructions of small objects have been reported at atomic resolution 4,5 , resolution places fundamental limitations to object-size. For larger objects (> 20 nm), the Crowther condition 1,6 discussed below typically limits volumetric resolutions of electron tomography to roughly 1 nm-twenty times worse than the best resolution in 2D projections. In addition, high-resolution (< 1 nm) tomography of general extended objects, to date, has not been possible with aberration-corrected instruments because the depth-of-field (5 -10 nm) of aberration-corrected STEMs is smaller than most objects of interest today 7 . High-resolution 3D reconstruction of extended objects, i.e. those larger than the depth-of-field, requires collecting information beyond a traditional tilt series. Here we present through-focal tomography that combines depth sectioning and traditional tilt-tomography to reconstruct extended objects, with highresolution, in three-dimensions. This combined approach fills in missing 3D information by acquiring a through-focal image series at each specimen tilt (Fig. 1)-decoupling the limiting Crowther relationship between 3D resolution and object size.For traditional (S)TEM tomography the images at every tilt-angle must correspond to a perfect projection of the original object to fulfill the "projection requ...