Direct Evidence of a Near-Ideal Jeff = 1/2 Ground State in Triangular-Lattice Na2BaCo(PO4)2

TL;DR

This study provides direct experimental evidence that Na2BaCo(PO4)2 hosts a near-ideal Jeff = 1/2 ground state due to minimal trigonal distortion, making it a promising system for exploring exotic magnetic phenomena.

Contribution

The paper combines polarization-dependent XAS and cluster calculations to demonstrate the near-ideal Jeff = 1/2 ground state in Na2BaCo(PO4)2 with minimal trigonal distortion.

Findings

Very small trigonal distortion of 11 meV in CoO6 octahedra

Close to ideal Jeff = 1/2 ground state achieved

Magnetic susceptibility consistent with theoretical model

Abstract

We investigated the local Co 3d electronic structure of Na2BaCo(PO4)2 using polarization-dependent X-ray absorption spectroscopy (XAS) in combination with full multiplet cluster calculations. We employed the line-fitting inverse partial fluorescence yield (IPFY) technique to obtain accurate XAS spectra from strong insulating materials. Our combined experimental and theoretical analysis reveals a very small effective trigonal distortion of only 11 meV in the CoO6 octahedra, indicating a close to ideal condition to render a ground state with the Jeff = 1/2 character. With our cluster model we were also able to simulate magnetic susceptibility measurements along different directions in the crystal. These findings highlight Na2BaCo(PO4)2 as a promising platform for exploring exotic magnetic phenomena associated with Jeff = 1/2 ground states on triangular lattices.