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Nitrogen represents an archetypal example of material exhibiting a pressuredriven transformation from molecular to polymeric state. Detailedinvestigations of such transformations are challenging because of a largekinetic barrier between molecular and polymeric structures, making thetransformation largely dependent on kinetic stimuli. In the case of nitrogen,additional complications occur due to the rich polymorphism in the vicinity ofthe transition. Here, we report the observation of both molecular (\theta) andpolymeric (BP) phases, crystallized upon temperature quenching of fluidnitrogen to room temperature at 97-114 GPa. Synchrotron single-crystal X-raydiffraction, Raman spectroscopy, and first-principles theoretical calculationshave been used for diagnostics of the phases and determination of theirstructure and stability. Molecular \theta-nitrogen is the most stable amongmolecular phases bordering the stability field of polymeric phases, partiallysettling a previously noted discrepancy between theory and experimentconcerning the thermodynamic stability limit of molecular phases.

Structural diversity of molecular nitrogen on approach to polymeric states