Electric field strength-dependent accuracy of TiAlN thin film composition measurements by laser-assisted atom probe tomography

Accurate quantification of absolute concentrations represents a major challenge for atom probe tomography (APT) since the field evaporation process is affected significantly by the measurement parameters. In the present work we investigate systematically the effect of laser pulse parameters on the accuracy of laser-assisted APT for a TiAlN thin film previously quantified by ion beam analysis, combining Rutherford backscattering spectrometry and time-of-flight elastic recoil detection analysis. The electric field strength is estimated from the Al²⁺/Al⁺ charge state ratio for all systematically varied measurement parameters. Subsequently, the absolute concentrations from laser-assisted APT are compared to ion beam analysis data. An increase of the electric field strength from approximately 25–28 V nm⁻¹ improves the accuracy of absolute concentrations measured by laser-assisted APT from 11.4 to 4.1 at% for N, from 8.8 to 3.0 at% for Al and from 2.8 to 0.9 at% for Ti. Our data emphasize that the measurement accuracy of laser-assisted APT for TiAlN is governed by the electric field strength. It is shown that the smallest compositional discrepancies between ion beam analysis and APT are obtained for the maximum electric field strength of approximately 28 V nm⁻¹ at 10 pJ laser pulse energy. This can be rationalized by considering the enhanced ionization of neutral fragments caused by the increased electric field strength. (paper)