Ba$_{3}$M$_{x}$Ti$_{3-x}$O$_{9}$(M = Ir, Rh): A family of 5\textit{\textcolor{black}{d}}/4\textit{\textcolor{black}{d}}-based, diluted quantum spin liquids

TL;DR

This study investigates a family of layered transition metal oxides with diluted magnetic ions, revealing evidence for quantum spin liquid states in Rh and Ir based compounds through structural, magnetic, and thermodynamic analyses.

Contribution

It reports the synthesis and characterization of new Ba$_{3}$M$_{x}$Ti$_{3-x}$O$_{9}$ compounds, demonstrating their potential as quantum spin liquids due to the absence of magnetic order down to very low temperatures.

Findings

Strong antiferromagnetic interactions observed.

No spin-freezing or magnetic order detected down to 0.35 K.

Quantum spin liquid behavior proposed for specific compositions.

Abstract

We report the structural and magnetic properties of the 4}\textit{\textcolor{black}{d }}\textcolor{black}{(M = Rh) based and 5}\textit{\textcolor{black}{d }}\textcolor{black}{(M = Ir) based systems Ba$_{3}$M$_{x}$Ti$_{3-x}$O$_{9}$ (nominally $x$ = 0.5, 1). The studied compositions were found to crystallize in a hexagonal structure with the centrosymmetric space group }$P6_{3}/mmc$.\textcolor{black}{{} The structures comprise of A$_{2}$O$_{9}$ polyhedra (with the A site (possibly) statistically occupied by M and Ti) in which pairs of transition metal ions are stacked along the crystallographic }\textit{\textcolor{black}{c}}\textcolor{black}{-axis. These pairs form triangular bilayers in the $ab$-plane. The magnetic Rh and Ir ions occupy these bilayers, diluted by Ti ions even for $x$ = 1. These bilayers are separated by a triangular layer which is dominantly occupied by Ti ions. From magnetization measurements we infer strong antiferromagnetic couplings for all of the materials but the absence of any spin-freezing or spin-ordering down to 2~K. Further, specific heat measurements down to 0.35~K show no sign of a phase transition for any of the compounds. Based on these thermodynamic measurements we propose the emergence of a quantum spin liquid ground state for Ba$_{3}$Rh$_{0.5}$Ti$_{2.5}$O$_{9}$, and Ba$_{3}$Ir$_{0.5}$Ti$_{2.5}$O$_{9}$, in addition to the already reported Ba$_{3}$IrTi$_{2}$O$_{9}$. }