PNAS

Flat-band tuning and emergent itinerant magnetism in Sr(Co 1− x Pd x ) 2 As 2

2025-12-17

The interplay between magnetism and flat-band (FB) instability is a central theme in quantum materials research. A striking example is the emergence of magnetic order in a nominally nonmagnetic compound when a flat band is tuned near the Fermi energy ( E F ). In this study, we investigate this phenomenon in the Pauli paramagnet SrCo 2 As 2 , where an FB associated with Co e g orbitals lies close to E F . Remarkably, a minute substitution of the nonmagnetic element Pd onto the Co site ( ∼ 2%) induces antiferromagnetic order with a transition temperature as high as T N = 25 K. Temperature- and magnetic-field-dependent magnetic and transport measurements, complemented by zero-field neutron diffraction, reveal a helical magnetic order for x ≤ 0.10 in Sr(Co 1− x Pd x ) 2 As 2 , transitioning to a complex ferromagnetic state at higher Pd concentrations. Spectroscopic evidence and theoretical band structure calculations demonstrate that electron doping shifts the flat band closer to E F , significantly enhancing the Stoner parameter. This enhancement drives a strong ferromagnetic instability, leading to helical magnetic ordering dominated by in-plane ferromagnetic interactions. The emergence of robust magnetic ordering through substitution with nonmagnetic elements is a unique phenomenon that underscores the pivotal role of flat-band instability in tuning magnetism in itinerant systems.

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DOI https://doi.org/10.1073/pnas.2519523122