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Two-dimensional (2D) transition metal nitrides (TMNs) are new members in the2D materials family with a wide range of applications. Particularly, highlycrystalline and large area thin films of TMNs are potentially promising forapplications in electronic and optoelectronic devices; however, the synthesisof such TMNs has not yet been achieved. Here, we report the synthesis offew-nanometer thin Mo5N6 crystals with large area and high quality via in situchemical conversion of layered MoS2 crystals. The structure and quality of theultrathin Mo5N6 crystal are confirmed using transmission electron microscopy,Raman spectroscopy and X-ray photoelectron spectroscopy. The large lateraldimensions of Mo5N6 crystals are inherited from the MoS2 crystals that are usedfor the conversion. Atomic force microscopy characterization reveals thethickness of Mo5N6 crystals is reduced to about 1/3 of the MoS2 crystal.Electrical measurements show the obtained Mo5N6 samples are metallic with highelectrical conductivity (~ 100 {\Omega} sq-1), which is comparable to graphene.The versatility of this general approach is demonstrated by expanding themethod to synthesize W5N6 and TiN. Our strategy offers a new direction forpreparing 2D TMNs with desirable characteristics, opening a door for studyingfundamental physics and facilitating the development of next generationelectronics.

Realization of 2D Crystalline Metal Nitrides via Selective Atomic Substitution