Magnetic and electronic ordering phenomena in the [Ru$_2$O$_6$] honeycomb lattice compound AgRuO$_3$

TL;DR

This study investigates the magnetic, electronic, and structural properties of AgRuO$_3$, revealing a high-temperature antiferromagnetic transition, complex conduction mechanisms, and insights into its magnetic structure through experimental and computational methods.

Contribution

It provides the first detailed characterization of AgRuO$_3$'s magnetic and electronic properties, including neutron diffraction and DFT calculations, highlighting similarities and differences with related compounds.

Findings

Sharp antiferromagnetic transition at 342 K

Conduction involves activated semiconducting gap and defect-related carriers

Magnetic structure is Néel-type with moments along the c axis

Abstract

The silver ruthenium oxide AgRuO$_3$ consists of honeycomb [Ru$_2^{5+}$O$_6^{2-}$] layers, and can be considered an analogue of SrRu$_2$O$_6$ with a different intercalation stage. We present measurements of magnetic susceptibility and specific heat on AgRuO$_3$ single crystals which reveal a sharp antiferromagnetic transition at 342(3)K. The electrical transport in single crystals of AgRuO$_3$ is determined by a combination of activated conduction over an intrinsic semiconducting gap of $\approx$ 100 meV and carriers trapped and thermally released from defects. From powder neutron diffraction data a N\'eel-type antiferromagnetic structure with the Ru moments along the $c$ axis is derived. Raman and muon spin rotation spectroscopy measurements on AgRuO$_3$ powder samples indicate a further weak phase transition or a crossover in the temperature range 125-200 K. The transition does not show up in magnetic susceptibility and its origin is argued to be related to defects but cannot be fully clarified. The experimental findings are complemented by DFT-based electronic structure calculations. It is found that the magnetism in AgRuO$_3$ is similar to that of SrRu$_2$O$_6$, however with stronger intralayer and weaker interlayer magnetic exchange interactions.