Role of Fe intercalation on the electronic correlation in resistively switchable antiferromagnet Fe$_{x}$NbS$_2$
Wenxin Li, Jonathan T. Reichanadter, Shan Wu, Ji Seop Oh, Rourav Basak, Shannon C. Haley, Elio Vescovo, Donghui Lu, Makoto Hashimoto, Christoph Klewe, Suchismita Sarker, James G. Analytis, Robert J. Birgeneau, Jeffrey B. Neaton, Yu He
公開日: 2025/9/3
Abstract
Among the family of intercalated transition-metal dichalcogenides (TMDs), Fe$_{x}$NbS$_2$ is found to possess unique current-induced resistive switching behaviors, tunable antiferromagnetic states, and a commensurate charge order, all of which are tied to a critical Fe doping of $x_c$ = 1/3. However, the electronic origin of such extreme stoichiometry sensitivities remains unclear. Combining angle-resolved photoemission spectroscopy (ARPES) with density functional theory (DFT) calculations, we identify and characterize a dramatic eV-scale electronic restructuring that occurs across the $x_c$. Moment-carrying Fe 3$d_{z^2}$ electrons manifest as narrow bands within 200 meV to the Fermi level, distinct from other transition metal intercalated TMD magnets. This state strongly interacts with the itinerant electron in TMD layer, and rapidly loses coherence above $x_c$. These observations resemble the exceptional electronic and magnetic sensitivity of strongly correlated systems upon charge doping, shedding light on the important role of electronic correlation in magnetic TMDs.