Hydrogenated PdCoO2: A layered Metallic Oxide with Robust Room-Temperature Ferromagnetism

Di Tian#, Haotian Zheng#, Zewei Huang#, Sijie Wu, Pengcheng Li, Cong Li, Jianbing Zhang, Xinyu Shu, Jinling Zhou, Yang Liu, Yanhong Gu, Meng Wang, Di Yi, Tianxiang Nan, Zhen Chen, Qing He, Huaqiang Wu, Shuyun Zhou, Weidong Luo*, Pu Yu*

2025 Physical Review X 15, 041030

Abstract

Layered oxide materials, with their two-dimensional crystalline architectures and tunable interlayer interaction, serve as a fertile field for harnessing emergent quantum phenomena. Among these materials, metallic delafossites (e.g., PdCoO 2 ) have emerged as a prominent system with extraordinary two-dimensional electronic properties, though their intrinsic lack of ferromagnetism has remained a fundamental constraint. Here, we report the creation of robust, bulk high-temperature ferromagnetism ( T c > 420 K ) in inherently nonmagnetic PdCoO 2 through controlled hydrogenation while preserving the delafossite structure. This process induces layer-selective electron doping into CoO 2 layers, stabilizing Ising-type ferromagnetism with pronounced perpendicular magnetic anisotropy while preserving the material’s exceptional metallicity. Remarkably, the system self-assembles into a superlattice of alternating metallic Pd and insulating ferromagnetic hydrogenated CoO 2 layers, enabling an unconventional anomalous Hall effect mediated by interlayer spin-charge coupling. These findings demonstrate that bulk ferromagnetism can be achieved in delafossite oxides while preserving their structural integrity, positioning hydrogenated delafossites as a versatile platform for exploring correlated quantum effects and designing multifunctional devices.

Research Topics

Magnetic Materials Functional Materials