Neutron Scattering Study of Magnetic Ordering and Excitations in the Doped Spin Gap System Tl(Cu$_{1-x}$Mg$_x$)Cl$_3$

TL;DR

This neutron scattering study reveals that doping TlCuCl3 with Mg induces antiferromagnetic order while preserving the spin gap, showing coexistence of magnetic order and spin gap states.

Contribution

The paper provides the first detailed neutron scattering analysis of impurity-induced magnetic order and excitations in doped TlCuCl3, demonstrating coexistence of order and spin gap.

Findings

Magnetic Bragg reflections observed below 3.45 K indicating antiferromagnetic order.

Triplet magnetic excitations and their dispersion relations determined.

Spin gap increases below the Néel temperature, indicating coexistence of order and spin gap.

Abstract

Neutron elastic and inelastic scattering measurements have been performed in order to investigate the spin structure and the magnetic excitations in the impurity-induced antiferromagnetic ordered phase of the doped spin gap system Tl(Cu$_{1-x}$Mg$_x$)Cl$_3$ with $x=0.03$. The magnetic Bragg reflections indicative of the ordering were observed at ${\pmb Q}=(h, 0, l)$ with integer $h$ and odd $l$ below $T_{\rm N}=3.45$ K. It was found that the spin structure of the impurity-induced antiferromagnetic ordered phase on average in Tl(Cu$_{1-x}$Mg$_x$)Cl$_3$ with $x=0.03$ is the same as that of the field-induced magnetic ordered phase for ${\pmb H} \parallel b$ in the parent compound TlCuCl$_3$. The triplet magnetic excitation was clearly observed in the $a^*$-$c^*$ plane and the dispersion relations of the triplet excitation were determined along four different directions. The lowest triplet excitation corresponding to the spin gap was observed at ${\pmb Q}=(h, 0, l)$ with integer $h$ and odd $l$, as observed in TlCuCl$_3$. It was also found that the spin gap increases steeply below $T_{\rm N}$ upon decreasing temperature. This strongly indicates that the impurity-induced antiferromagnetic ordering coexists with the spin gap state in Tl(Cu$_{1-x}$Mg$_x$)Cl$_3$ with $x=0.03$.