Atom probe tomography (APT) helps elucidate the link between the nanoscale chemical variations and physical properties, but it has a limited structural resolution. Field ion microscopy (FIM), a predecessor technique to APT, is capable of attaining atomic resolution along certain sets of crystallographic planes albeit at the expense of elemental identification. We demonstrate how two commercially available atom probe instruments, one with a straight flight path and one fitted with a reflectron lens, can be used to acquire time-of-flight mass spectrometry data concomitant with a FIM experiment. We outline various experimental protocols making the use of temporal and spatial correlations to best discriminate field-evaporated signals from the large field-ionized background signal, demonstrating an unsophisticated yet efficient data mining strategy to provide this discrimination. We discuss the remaining experimental challenges that need to be addressed, notably concerned with accurate detection and identification of individual field-evaporated ions contained within the high field-ionized flux that contributes to a FIM image. Our hybrid experimental approach can, in principle, exhibit true atomic resolution with elemental discrimination capabilities, neither of which atom probe nor FIM can individually fully deliver—thereby making this new approach, here broadly termed analytical field ion microscopy (aFIM), unique.

Although atom probe tomography (APT) reconstructions do not directly influence the local elemental analysis, any structural inferences from APT volumes demand a reliable reconstruction of the point cloud. Accurate estimation of the reconstruction parameters is crucial to obtain reliable spatial scaling. In the current work, a new automated approach of calibrating atom probe reconstructions is developed using only one correlative projection electron microscopy (EM) image. We employed an algorithm that implements a 2D cross-correlation of microstructural features observed in both the APT reconstructions and the corresponding EM image. We apply this protocol to calibrate reconstructions in a Cu(In,Ga)Se2-based semiconductor and in a Co-based superalloy. This work enables us to couple chemical precision to structural information with relative ease.