Assessing Advanced Methods in Xps and Haxpes for Determining the Thicknesses of High-K Oxide Materials: from Ultra-Thin Layers to Deeply Buried Interfaces

We assess advanced XPS-based methods in determining depth distribution in alumina and hafnia ALD samples of increasing thicknesses and buried layer depths. First, dose quantification of Al in ultrathin alumina is achieved through non-destructive wavelength dispersive X-ray fluorescence (WDXRF), which is confirmed by comparison to destructive liquid-phase deposition inductively coupled plasma mass spectrometry (LPD-ICPMS) (uncertainty 10 %). Second, we compare WDXRF to parallel ARXPS (pARXPS) in precise dose and thickness quantification in ultrathin alumina, and present the ability of pARXPS to accurately track linear growth during the deposition. Thickness determination of an intermediate ALD stack of silicon dioxide, hafnia, and alumina layers of 1-2 nm by pARXPS is evaluated against quantitative, reference-free grazing incidence X-ray fluorescence (GIXRF) (uncertainty 8-9 %). An alternative technique employing inelastic background analysis (IBA) is introduced as a fast and accurate method and subsequently compared with pARXPS and GIXRF thickness determinations. Finally, in thicker multilayer systems, hard X-ray photoelectron spectroscopy (HAXPES) combined with IBA is proposed for an in-depth analysis for thicknesses up to 28 nm, with generated interface locations and layer thicknesses wellaligned to nominal values. This study is a novel application of lab-based Cr-K alpha HAXPES spectra for inelastic background analysis in thick metal-oxide multilayer materials.