Kavli Affiliate: Jeffrey B. Neaton
| First 5 Authors: Wenxin Li, Wenxin Li, , ,
| Summary:
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.
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