Imprinting Ferromagnetism and Superconductivity in Single Atomic Layers of Molecular Superlattices
Zejun Li, Xiuying Zhang, Xiaoxu Zhao, Jing Li, Tun Seng Herng, Haomin Xu, Fanrong Lin, Pin Lyu, Xinnan Peng, Wei Yu, Xiao Hai, Cheng Chen, Huimin Yang, Jens Martin, Jing Lü, Jing Lü, Xin Luo, A. H. Castro Neto, Stephen J. Pennycook, Jun Ding, Yuan Ping Feng, Jiong Lu, Jiong Lu
Abstract
Abstract Ferromagnetism and superconductivity are two antagonistic phenomena since ferromagnetic exchange fields tend to destroy singlet Cooper pairs. Reconciliation of these two competing phases has been achieved in vertically stacked heterostructures where these two orders are confined in different layers. However, controllable integration of these two phases in one atomic layer is a longstanding challenge. Here, an interlayer‐space‐confined chemical design (ICCD) is reported for the synthesis of dilute single‐atom‐doped TaS 2 molecular superlattice, whereby ferromagnetism is observed in the superconducting TaS 2 layers. The intercalation of 2H‐TaS 2 crystal with bulky organic ammonium molecule expands its van der Waals gap for single‐atom doping via co‐intercalated cobalt ions, resulting in the formation of quasi‐monolayer Co‐doped TaS 2 superlattices. Isolated Co atoms are decorated in the basal plane of the TaS 2 via substituting the Ta atom or anchoring at a hollow site, wherein the orbital‐selected p–d hybridization between Co and neighboring Ta and S atoms induces local magnetic moments with strong ferromagnetic coupling. This ICCD approach can be applied to various metal ions, enabling the synthesis of a series of crystal‐size TaS 2 molecular superlattices.