Origin of a Topotactic Reduction Effect for Superconductivity in Infinite-Layer Nickelates
Shengwei Zeng, Chi Sin Tang, Zhaoyang Luo, L. E. Chow, Zhi Shiuh Lim, Saurav Prakash, Ping Yang, Caozheng Diao, Xiaojiang Yu, Zhenxiang Xing, Rong Ji, Xinmao Yin, Changjian Li, Xiao Renshaw Wang, Qian He, Mark B. H. Breese, Ariando Ariando, Huajun Liu
Abstract
Topotactic reduction utilizing metal hydrides as reagents has emerged as an effective approach to achieve exceptionally low oxidization states of metal ions and unconventional coordination networks. This method opens avenues to the development of entirely new functional materials, with one notable example being the infinite-layer nickelate superconductors. However, the reduction effect on the atomic reconstruction and electronic structures-crucial for superconductivity-remains largely unresolved. We designed two sets of control Nd_{0.8}Sr_{0.2}NiO_{2} thin films and used secondary ion mass spectroscopy to highlight the absence of reduction-induced hydrogen intercalation. X-ray absorption spectroscopy revealed a significant linear dichroism with dominant Ni 3d_{x2-y2} orbitals on superconducting samples, indicating a Ni single-band nature of infinite-layer nickelates. Consistent with the superconducting T_{c}, the Ni 3d orbitals asymmetry manifests a domelike dependence on the reduction duration. Our results unveil the critical role of reduction in modulating the Ni-3d orbital polarization and its impact on the superconducting properties.