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The ordered tetragonal intermetallic Cr$_2$Al forms the same structure typeas Mn$_2$Au, and the latter has been heavily investigated for its potential inantiferromagnetic spintronics due to its degenerate in-plane N\'{e}el vector.We present the single crystal flux growth of Cr$_2$Al and orientation-dependentmagnetic properties. Powder neutron diffraction of Cr$_2$Al andfirst-principles simulations reveal that the magnetic ordering is likelyin-plane and therefore identical to Mn$_2$Au, providing a second materialcandidate in the MoSi$_2$ structure type to evaluate the fundamentalinteractions that govern spintronic effects. The single ordering transitionseen in thermal analysis and resistivity indicates that no canting of themoments along the $c$ axis is likely. Magnetometry, resistivity, anddifferential scanning calorimetry measurements confirm the N\'{e}el temperatureto be $634 \pm 2$ K. First-principles simulations indicate that the system hasa small density of states at the Fermi energy and confirm the lowest-energymagnetic ground state ordering, while Monte Carlo simulations match theexperimental N\'{e}el temperature.

In-plane magnetic structure and exchange interactions in the high-temperature antiferromagnet Cr2Al