Mapping energetics of atom probe evaporation events through first principles calculations

The purpose of this work is to use atomistic modeling to determine accurate inputs into the atom probe tomography (APT) reconstruction process. One of these inputs is evaporation field; however, a challenge occurs because single ions and dimers have different evaporation fields. We have calculated the evaporation field of Al and Sc ions and Al–Al and Al–Sc dimers from an L12-Al3Sc surface using ab initio calculations and with a high electric field applied to the surface. The evaporation field is defined as the electric field at which the energy barrier size is calculated as zero, corresponding to the minimum field that atoms from the surface can break their bonds and evaporate from the surface. The evaporation field of the surface atoms are ranked from least to greatest as: Al–Al dimer, Al ion, Sc ion, and Al–Sc dimer. The first principles results were compared with experimental data in the form of an ion evaporation map, which maps multi-ion evaporations. From the ion evaporation map of L12-Al3Sc, we extract relative evaporation fields and identify that an Al–Al dimer has a lower evaporation field than an Al–Sc dimer. Additionally, comparatively an Al–Al surface dimer is more likely to evaporate as a dimer, while an Al–Sc surface dimer is more likely to evaporate as single ions. These conclusions from the experiment agree with the ab initio calculations, validating the use of this approach for modeling APT energetics.

► Calculated evaporation field of monomer and dimer atom probe evaporations.
► Determined relative evaporation fields using ion evaporation maps.
► Compared the experimental and calculated results and found that they agreed.