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Using modern crystal structure prediction program (CALYPSO), we searched manyexperimentally synthesizable low-energy structures with perfect or nearlyperfect easy-axis magnetocrystalline anisotropy energy (MAE) in manganesenitride, including MnN, Mn2N, Mn3N2, Mn5N2, Mn4N, respectively, which are themore frequently studied stoichiometries by experimental researchers. MnN (I-42d) shows giant MAE with values of E001=1006, E010=0, E100=920 ueV/atom(same hereinafter), respectively. One perfect easy-axis MAE in Mn3N2 (P42/mmc)with correspondent values of E010=E100=12 is observed, the other nearly perfecteasy-axis MAE one (Ibam) with respective values of E001=324 and E010=345 isobserved. Four almost totally perfect easy-axis MAE structures are obtained inMn2N, including P4/mmm with individual E001=249 and E100=250, Pccm withE001=E100=62, P4/nmm with E001=58 and E100=60, Imma with E001=108 and E100=109,respectively. Three structures including one perfect candidates are found inMn4N, including Fmmm with individual E001=126 and E010=121, I4/mmm withE010=127 and E100=133, I4/mmm with E001= E100=169, respectively. Too manyvaluable structures are deserved to be further studied by both theoretical andexperimental scientists. The present study might attract close attention tothese several compounds.

Predicting synthesizable manganese nitride with unprecedentedly giant magnetocrystalline anisotropy energy