Impact of Oxidation State on the Valence-bond-glass Physics in the lithium-intercalated Mo${}_3$O${}_8$ Cluster Mott Insulators

Abstract

We have successfully synthesized four Mo${}_3$O${}_8$-type cluster Mott insulators (CMI) by intercalating lithium into nonmagnetic precursors to regulate the Mo${}_3$ cluster valence. The resulting materials are Li${}_{1+x}$$R$Mo${}_3$O${}_8$ ($R$ = Sc, Y, Lu) and Li${}_x$Zn${}_2$Mo${}_3$O${}_8$. Our magnetic susceptibility measurements revealed that these materials display characteristics akin to a valence bond glass state and suggest the presence of short-range ordering when the Mo${}_3$ cluster valence approximates its ideal value. These findings challenge the prevailing belief that the plaquette charge ordering state is an inherent feature of Mo${}_3$O${}_8$-type CMI. Instead, they underscore the importance of Mo${}_3$ cluster valence in determining the physical properties of these systems. These insights furnish a fresh understanding of the Mo${}_3$O${}_8$-type CMI and open new research opportunities in highly frustrated magnetism.

13page, 11figures, manuscript accepted for publication in Physical Review B

References in corpus (8)

• Spin Dynamics of the Spin-1/2 Kagome Lattice Antiferromagnet ZnCu_3(OH)_6Cl_2
• Spin-Liquid State in the S = 1/2 Hyperkagome Antiferromagnet Na4Ir3O8
• Vesignieite BaCu3V2O8(OH)2 as a Candidate Spin-1/2 Kagome Antiferromagnet
• Possible valence-bond condensation in the frustrated cluster magnet LiZn2Mo3O8
• The Valence Bond Glass phase
• Electronic tunability of the frustrated triangular-lattice cluster magnet LiZn${}_{2-x}$Mo${}_3$O${}_8$
• Quantum magnetisms in uniform triangular lattices Li2AMo3O8 (A = In, Sc)
• Controlling the stoichiometry of the triangular lattice antiferromagnet Li${}_{1+x}$Zn${}_{2-y}$Mo${}_3$O${}_8$

Cited by in corpus (1)

• Magnetic ordering of the Mo${}_3$O${}_8$-type cluster Mott insulator Na${}_3$Sc${}_2$(MoO${}_4$)${}_2$Mo${}_3$O${}_8$ with spin-1/2 triangular lattice prepared via optimal synthesis