Band-Mott mixing hybridizes the gap in Fe${}_2$Mo${}_3$O${}_8$

Abstract

We combined optical spectroscopy and first principles electronic structure calculations to reveal the charge gap in the polar magnet Fe${}_2$Mo${}_3$O${}_8$. Iron occupation on the octahedral site draws the gap strongly downward compared to the Zn parent compound, and subsequent occupation of the tetrahedral site creates a narrow resonance near the Fermi energy that draws the gap downward even further. This resonance is a many-body effect that emanates from a flat valence band in a Mott-like state due to screening of the local moment - similar to expectations for a Zhang-Rice singlet, except that here, it appears in a semi-conductor. We discuss the unusual hybridization in terms of orbital occupation and character as well as the structure-property relationships that can be unveiled in various metal-substituted systems (Ni, Mn, Co, Zn).

References in corpus (5)

• Quantum Monte Carlo Impurity Solver for Cluster DMFT and Electronic Structure Calculations in Adjustable Base
• Orbital selective Mott transition in multi-band systems: slave-spin representation and dynamical mean-field theory
• Possible valence-bond condensation in the frustrated cluster magnet LiZn2Mo3O8
• Picosecond creation of switchable optomagnets with giant photoinduced Kerr rotations in polar antiferromagnetic (Fe${}_{1-x}$Zn${}_x$)${}_2$Mo${}_3$O${}_8$
• Ordering of Fe and Zn ions and magnetic properties of FeZnMo3O8

Cited by in corpus (6)

• Colossal linear magnetoelectricity in polar magnet Fe2Mo3O8
• Noncollinear magnetic order, in-plane anisotropy, and magnetoelectric coupling in a pyroelectric honeycomb antiferromagnet Ni${}_2$Mo${}_3$O${}_8$
• Optical magnetoelectric effect in the polar honeycomb antiferromagnet Fe2Mo3O8
• Electronic structure of the frustrated diamond lattice magnet NiRh${}_2$O${}_4$
• Antiferromagnetic to Ferrimagnetic Phase Transition and Possible Phase Coexistence in Polar Magnets (Fe${}_{1-x}$Mn${}_x$)${}_2$Mo${}_3$O${}_8$
• Controlled growth of polar altermagnets via chemical vapor transport