Valence bond glass state in the 4$d^1$ fcc antiferromagnet Ba$_2$LuMoO$_6$

TL;DR

This study reveals that Ba$_2$LuMoO$_6$, a 4$d^1$ double perovskite, exhibits a valence bond glass state with dynamic magnetism down to very low temperatures, distinguished from 5$d^1$ counterparts.

Contribution

It provides the first detailed investigation of Ba$_2$LuMoO$_6$, demonstrating its valence bond glass ground state through muon spectroscopy and neutron scattering.

Findings

Magnetism remains dynamic down to 60 mK without spin freezing.

A singlet-triplet excitation gap of 28 meV was observed.

The ground state is similar to that of Ba$_2$YMoO$_6$, indicating a valence bond glass.

Abstract

$B$-site ordered 4$d^1$ and 5$d^1$ double perovskites have a number of potential novel ground states including multipolar order, quantum spin liquids and valence bond glass states. These arise from the complex interactions of spin-orbital entangled $J_{eff}$ = 3/2 pseudospins on the geometrically frustrated fcc lattice. The 4$d^1$ Mo$^{5+}$ perovskite Ba$_2$YMoO$_6$ has been suggested to have a valence bond glass ground state. Here we report on the low temperature properties of powder samples of isostructural Ba$_2$LuMoO$_6$: the only other known cubic 4$d^1$ perovskite with one magnetic cation. Our muon spectroscopy experiments show that magnetism in this material remains dynamic down to 60 mK without any spin freezing or magnetic order. A singlet-triplet excitation with a gap of $\Delta$ = 28 meV is observed in inelastic neutron scattering. These results are interpreted as a disordered valence bond glass ground state similar to Ba$_2$YMoO$_6$. Our results highlight the differences of the 4$d^1$ double perovskites in comparison to cubic 5$d^1$ analogues, which have both magnetic and multipolar order.