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The interface of a La0.7Sr0.3MnO3/SrTiO3 bilayer was modulated by introducing 3 unit cells of Ba1-xSrxTiO3 using Combinatorial Pulsed Laser Deposition. A wide range of chemical compositions was studied within the same sample, with BSTx stoichiometry variable from 0.5 to 1 along Y-axis, while the SrTiO3 overlayer thickness was modified along the X direction [Fig. 1(a)]. We performed high-resolution, laboratory-based angle-resolved XPS studies of the BSTx film surface providing information on the thickness and composition of the surface and sub-surface layers. Based on the attenuation of the La 3d corelevel photoemission signal from the La0.7Sr0.3MnO3 bottom layer, the BST layer is 1.2 nm thick. XPS Ba 3d5/2 core-level spectra were acquired at positions corresponding to different nominal Ba/Sr stoichiometry. In all measurements, the Ba 3d5/2 core-level spectra can be represented by two main components, i.e. one component at higher binding energy (BE = 780.54 eV) corresponding to surface contribution and the other one at lower binding energy (BE = 778.92 eV) corresponding to sub-surface contribution (Figs. 2 and 3). Going from normal to 60° emission angle and using a 3-unit cell thick film model, the surface to sub-surface intensity ratio clearly evolves providing evidence of a Ba-rich surfactant. The surfactant effect is more significant for lower nominal Ba stoichiometry.

We have studied the field cycling behavior of microscopic TiN/Hf0.5Zr0.5O2/TiN ferroelectric capacitors using synchrotron-based soft x-ray photoemission electron microscopy. The oxygen vacancy ( V O ) concentration near the top TiN/Hf0.5Zr0.5O2 interface is estimated from the reduction of Hf4+ to Hf3+ as measured in the Hf 4f core level spectra. The V O concentration increases with field cycling and redistributes under the effect of the internal field due to the polarization. Upward pointing polarization slightly depletes the concentration near the top interface, whereas downward polarization causes V O drift toward the top interface. The V O redistribution after wake-up is consistent with shifts in the I–V switching peak. The Schottky barrier height for electrons decreases systematically with cycling in polarization states, reflecting the overall increase in V O . [ABSTRACT FROM AUTHOR]