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Non-metal nitrides are an exciting field of chemistry, featuring asignificant number of compounds that can possess outstanding materialproperties. This characteristic relies on maximizing the number of strongcovalent bonds, with crosslinked XN6 octahedra frameworks being particularlyintriguing. In this study, the phosphorus-nitrogen system was studied up to 137GPa in laser-heated diamond anvil cells and three previously unobserved phaseswere synthesized and characterized by single-crystal X-ray diffraction, Ramanspectroscopy measurements and density functional theory calculations.Delta-P3N5 and PN2 were found to form at 72 and 134 GPa, respectively, and bothfeature dense 3D networks of the so far elusive PN6 units. The two areultra-incompressible, having a bulk modulus of K0 = 322 GPa for delta-P3N5 andK0 = 339 GPa for PN2. Upon decompression below 7 GPa, delta-P3N5 undergoes atransformation into a novel alpha'-P3N5 solid, stable at ambient conditions,that has a unique structure type based on PN4 tetrahedra. The formation ofalpha'-P3N5 underlines that a phase space otherwise inaccessible can beexplored through high-pressure formed phases.

Revealing Phosphorus Nitrides up to the Megabar Regime: Synthesis of alpha-P3N5, delta-P3N5 and PN2