Structural and Magnetic Phase Transitions in Chromium Nitride Thin Films Grown by RF Nitrogen Plasma Molecular Beam Epitaxy

A magneto-structural phase transition is investigated in single crystal CrN thin films grown by rf plasma molecular beam epitaxy on MgO(001) substrates. While still within the vacuum environment following MBE growth, $in-situ$ low-temperature scanning tunneling microscopy, and $in-situ$ variable low-temperature reflection high energy electron diffraction are applied, revealing an atomically smooth and metallic CrN(001) surface, and an $\it in-plane$structuraltransitionfrom1$\times$1(primitiveCrNunitcell)to$$\sqrt{2}\times \sqrt{2}-\mathrm{R}{45}^{\circ }$$withatransitiontemperatureof$\sim$278K,respectively\mathrm{.}$\it Ex-situ$ temperature dependent measurements are also performed, including x-ray diffraction and neutron diffraction, looking at the structural peaks and likewise revealing a first-order structural transition along both [001] and [111] $out-of-plane$ directions, with transition temperatures of 256 K and 268 K, respectively. Turning to the magnetic peaks, neutron diffraction confirms a clear magnetic transition from paramagnetic at room temperature to antiferromagnetic at low temperatures with a sharp, first-order phase transition and a N$\acute{e}$el temperature of 270 K or 280 K for two different films. In addition to the experimental measurements of structural and magnetic ordering, we also discuss results from first-principles theoretical calculations which explore various possible magneto-structural models.