The Dynamic Atom-Probe: Past, Present, and Perspectives.

Abstract

The present communication aims at demonstrating the wealth of information accessible by 1D-atom probe experiments using pulsed field desorption mass spectrometry (PFDMS), ultimately combined with video-field ion microscopy, while subjecting metallic samples to elevated gas pressures and studying surface reaction kinetics. Two case studies are being presented here: (a) the microkinetics of nickel tetracarbonyl (Ni(CO)4) formation through reaction of carbon monoxide with nickel and (b) the nitric oxide decomposition and reaction with hydrogen on platinum at variable steady electric fields mimicking electrocatalytic conditions. In both cases, surface areas with 140-150 atomic sites of the stepped Ni (001) and Pt (111) sample surfaces were probed. Under (a), we demonstrate variable repetition frequencies of field pulses to inform kinetic and mechanistic details of the surface reaction while under (b), we reveal the occurrence of field-induced processes impacting the surface reaction mechanism of nitric oxide with hydrogen and therefore opening new pathways not available under purely thermal conditions (in the absence of electric fields). Some aspects of PFDMS technical achievements will be discussed as they may provide clues for designing dynamic atom probe tomography instrumentation.