Tuning magnetic, lattice, and transport properties in CoNb3S6 via Fe doping

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We present a comprehensive investigation of the effects of Fe doping on the lattice dynamics, magnetic ordering, and magneto-transport properties of the intercalated van der Waals antiferromagnets Co1-xFexNb3S6 (x = 0.1 and 0.3). Temperature- and polarization-dependent Raman scattering measurements reveal a pronounced blue shift of the 180 cm-1 phonon mode with increasing Fe concentration, indicating enhanced sensitivity of lattice vibrations to Fe-induced structural and mass effects. While the temperature evolution of the phonon modes is dominated by conventional anharmonic phonon softening, subtle anomalies observed near the Néel temperature for x = 0.1 point to weak spin-phonon coupling. Electrical transport and magnetic susceptibility data show clear signatures of the antiferromagnetic phase transitions at TN ~ 20.5-23.7 K for x = 0.1 and TN ~ 32.0 K for x = 0.3. Out-of-plane magnetization measurements reveal hysteretic behavior with two field-induced transitions for x =0.1, which evolve into a single hysteresis loop at x =0.3, signaling a subtle reconstruction of the magnetic ground state. Magneto-transport measurements for x = 0.1 further display a butterfly-shaped hysteretic magnetoresistance and a weak topological Hall effect; however, both features are strongly suppressed at x = 0.3. These results illustrate the critical role of Fe-induced magnetic structure reconstruction in fine-tuning topological and magnetic transport phenomena in intercalated van der Waals antiferromagnets.

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