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Whether {\alpha}double prime-Fe16N2 possesses a giant saturationmagnetization (Ms) has been a daunting problem among magnetic researchers foralmost 40 years, mainly due to the unshakable faith of famous Slater-Pauling(SP) curve and poor consistency on evaluating its Ms. Here we demonstrate that,using epitaxy and mis-fit strain imposed by an underlying substrate, thein-plane lattice constant of Fe16N2 thin films can be fine tuned to createfavorable conditions for exceptionally large saturation magnetization. Combinedstudy using polarized neutron reflectometry and X-ray diffraction shows thatwith increasing strain at the interface the Ms of these film can be changedover a broad range, from ~2.1T (non-high Ms) up to ~3.1T (high Ms). We suggestthat the equilibrium in-plane lattice constant of Fe16N2 sits in the vicinityof the spin crossover point, in which a transition between low spin to highspin configuration of Fe sites can be realized with sensitive adjustment ofcrystal structure.

Giant saturation magnetization effect in epitaxial Fe16N2 thin films grown on MgO (001) substrate