Magnetic properties and revisited exchange integrals of the frustrated chain cuprate PbCuSO$_4$(OH)$_2$ - linarite

TL;DR

This study investigates the magnetic properties of the frustrated chain cuprate linarite, revealing anisotropic saturation fields, larger exchange interactions than previously reported, and evidence of strong magnetic frustration with correlations above the ordering temperature.

Contribution

The paper provides revised exchange integrals for linarite using multiple experimental and theoretical approaches, shifting the frustration ratio closer to the critical point and enhancing understanding of its magnetic behavior.

Findings

Anisotropic saturation fields along main axes.

Larger exchange interactions J1 and J2 than previous studies.

Evidence of magnetic frustration and correlations above T_N.

Abstract

We present a detailed study in the paramagnetic regime of the frustrated $s$ = 1/2 spin-compound linarite, PbCuSO$_4$(OH)$_2$, with competing ferromagnetic nearest-neighbor and antiferromagnetic next-nearest-neighbor exchange interactions. Our data reveal highly anisotropic values for the saturation field along the crystallographic main directions, with $\sim$ 7.6, $\sim$ 10.5 and $\sim$ 8.5\,T for the $a$, $b$, and $c$ axes, respectively. In the paramagnetic regime, this behavior is explained mainly by the anisotropy of the \textit{g}-factor but leaving room for an easy-axis exchange anisotropy. Within the isotropic $J_1$-$J_2$ spin model our experimental data are described by various theoretical approaches yielding values for the exchange interactions $J_1$ $\sim$ -100\,K and $J_2$ $\sim$ 36\,K. These main intrachain exchange integrals are significantly larger as compared to the values derived in two previous studies in the literature and shift the frustration ratio $\alpha = J_2/|J_1|$ $\approx$ 0.36 of linarite closer to the 1D critical point at 0.25. Electron spin resonance (ESR) and nuclear magnetic resonance (NMR) measurements further prove that the static susceptibility is dominated by the intrinsic spin susceptibility. The Knight shift as well as the broadening of the linewidth in ESR and NMR at elevated temperatures indicate a highly frustrated system with the onset of magnetic correlations far above the magnetic ordering temperature $T_\mathrm{N}$ = 2.75(5)\,K, in agreement with the calculated exchange constants.