Impact of Polarity Mismatch in Infinite-Layer Nickelates

The recent discovery of superconductivity in infinite-layer Sr-doped NdNiO2 grown on SrTiO3(001) provides a new platform to explore the conducting mechanism of unconventional superconductors. However, the electronic structure of infinite-layer nickelates remains controversial. In this paper, we systematically compare the structural and electronic properties of NdNiO2 films grown on SrTiO3 and LaAlO3 substrates using first-principles calculations. Our results show that the lattice reconstruction accompanied by electronic reconstruction occurs in nickelate films on both substrates. Although both heterostructures (HSs) are conducting at the interface, the SrTiO3-based HS shows distinct atomic displacement in the interfacial TiO2 layer and significant electron accumulation deep into three SrTiO3 layers below the interface, while the LaAlO3-based HS shows negligible atomic displacement and electron localization in the interfacial AlO2 layer, reflecting the impact of polarity mismatch on the electronic structure. Further, Wannier function calculations reveal that the interface stress has no obvious effect on the splitting energy and hopping integral between Ni 3d and Nd-layer orbitals. Although the hybridization between Ni 3d (2)(x)-y(2) and Nd 5d orbitals is tiny, the hybridization between the Ni 3d (2)(x)-y(2) orbital and an itinerant interstitial s (IIS) orbital is significantly strong in both cases, suggesting that the IIS orbital may play a critical role in the superconductivity of nickelates.