Scanning tunnelling microscopy and X-ray photoemission studies of NdNiO2 infinite-layer nickelates films

Abstract: We report scanning tunnelling microscopy (STM) and x-ray photoemission spectroscopy (XPS) measurements on uncapped and SrTiO3 (STO) capped NdNiO2 realized by pulsed-laser deposition and topotactic reduction process. We find that untreated NdNiO2 surfaces are insulating and contain Ni mostly in a nominal Ni2+ oxidation state. Room temperature STM shows signatures of a striped-like topographic pattern, possibly compatible with recent reports of ordered oxygen vacancies in uncapped nickelates due to incomplete oxygen de-intercalation of the upper layers. A metallic surface and a full Ni1+ oxidation state is recovered by ultra high vacuum annealing at 250 C, as shown by STM and XPS. STO-capped NdNiO2 films, on the other hand, show Ni mostly in Ni1+ configuration, but Nd 3d5/2 core level spectra have a relevant contribution from ligand 4f 4L states, suggesting the formation of a NdTiNiOx layer at the interface with the STO. By in situ unit-cell by unit-cell Ar-ion sputtering removal of the STO capping and of the non stoichiometric interface layer, we were able to address the surface electronic properties of these samples, as shown by high resolution valence band photoemission spectroscopy. The results provide insights in the properties of infinite-layer NdNiO2 thin films prepared by the CaH2 topotactic reduction of perovskite NdNiO3 and suggest methods to improve their surface quality.