ArXiv · 2026
In itinerant magnets governed by the Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction, the exchange coupling depends on both the moment-moment distance r and the Fermi wavevector k_F, yet in bulk synthesis the two are tightly coupled: a change in composition typically alters both. Here, we use a thin-film approach to tune these two variables independently in a single crystalline host. Using molecular-beam epitaxy (MBE), we stabilize either 2×2R0^∘ Cr_(1/4)NbSe₂ or √3×√3R30^∘ Cr_(1/3)NbSe₂ within the same NbSe₂ host through separate growth windows. Controlled post-growth annealing performed across a series of temperatures then modifies the carrier density while leaving the Cr superstructure intact below a structural-transition threshold. The two as-grown phases are distinct in electronic structure, magnetic ground state, and transport. Along this annealing series, the Hall response evolves systematically while the magnetic response changes in a structurally insensitive manner, with ferromagnetic order emerging within the same √3×√3R30^∘ structural class only above a critical annealing temperature, experimentally disentangling carrier density and moment geometry. The Hall magnitude and sign evolution point to a low-carrier-density system in which k_F is susceptible to modest external tuning. Cr-NbSe₂ thus realizes carrier-sensitive RKKY magnetism in a single crystalline host, within an MBE-plus-annealing approach extensible across the intercalated transition-metal dichalcogenide family.
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