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Field evaporation from ionic or covalently bonded materials often leads tothe emission of molecular ions. The metastability of these molecular ions,particularly under the influence of the intense electrostatic field (1010Vm-1), makes them prone to dissociation with or without an exchange of energyamongst them. These processes can affect the analytical performance of atomprobe tomography (APT). For instance, neutral species formed throughdissociation may not be detected at all or with a time of flight no longerrelated to their mass, causing their loss from the analysis. Here, we evaluatedthe changes in the measured composition of FeO, Fe2O3 and Fe3O4 across a widerange of analysis conditions. Possible dissociation reactions are predicted bydensity-functional theory (DFT) calculations considering the spin states of themolecules. The energetically favoured reactions are traced on to the multi-hition correlation histograms, to confirm their existence within experiments,using an automated Python-based routine. The detected reactions are carefullyanalysed to reflect upon the influence of these neutrals from dissociationreactions on the performance of APT for analysing iron oxides.

Understanding atom probe's analytical performance for iron oxides using correlation histograms and ab initio calculations