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Eu$_5$In$_2$Sb$_6$ is an orthorhombic non-symmorphic small band gapsemiconductor with three distinct Eu$^{2+}$ sites and two low-temperaturemagnetic phase transitions. The material displays one of the greatest(negative) magnetoresistances of known stoichiometric antiferromagnets andbelongs to a family of Zintl materials that may host an axion insulator. Usingsingle crystal neutron diffraction, we show that the$T_{\mathrm{N1}}=14\mathrm{~K}$ second-order phase transition is associatedwith long-range antiferromagnetic order within the chemical unit cell $\left(k_1 = (000) \right)$. Upon cooling below $T_{\mathrm{N1}}$, the relativesublattice magnetizations of this structure vary until a second-order phasetransition at $T_{\mathrm{N2}}=7\mathrm{~K}$ that doubles the unit cell alongthe $\hat{c}$ axis $\left( k_2 = \left(00\frac{1}{2}\right) \right)$. We showthe anisotropic susceptibility and our magnetic neutron diffraction data areconsistent with magnetic structures described by the $\Gamma_3$ irreduciblerepresentation with the staggered magnetization of the $k_1$ and $k_2$components polarized along the $\hat{b}$ and $\hat{a}$ axis, respectively. Asthe $k_2$ component develops, the amplitude of the $k_1$ component is reduced,which indicates a 2k non-collinear magnetic structure. Density functionaltheory is used to calculate the energies of these magnetic structures and toshow the $k_1$ phase is a metal so $T_{\mathrm{N1}}$ is a rare example of aunit-cell-preserving second-order phase transition from a paramagneticsemiconductor to an antiferromagnetic metal. DFT indicates the transition at$T_{\mathrm{N2}}$ to a doubled unit cell reduces the carrier density of themetal, which is consistent with resistivity data.

Non-collinear 2k antiferromagnetism in the Zintl semiconductor Eu$_5$In$_2$Sb$_6$