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Search of materials with C-N composition hold a great promise in creatingmaterials which would rival diamond in hardness due to the very strong andrelatively low-ionic C-N bond. Early experimental and theoretical works on C-Ncompounds were based on structural similarity with binary A3B4 structural-types; however, the synthesis of C3N4 remains elusive. Here we explored anunbiased synthesis from the elemental materials at high pressures andtemperatures. Using in situ synchrotron X-ray diffraction and Ramanspectroscopy we demonstrate synthesis of highly incompressible Pnnm CN compoundwith sp3 hybridized carbon is synthesized above 55 GPa and 7000 K. This resultis supported by first principles evolutionary search, which finds that Pnnm CNis the most stable compound above 10.9 GPa. On pressure release below 6 GPa thesynthesized CN compound amorphizes reattaining its 1:1 stoichiometry asconfirmed by Energy-Dispersive X-ray Spectroscopy. This work underscores theimportance of understanding of novel high-pressure chemistry rules and it opensa new route for synthesis of superhard materials.

Synthesis of ultra-incompressible sp3-hybridized carbon nitride