Abstract
Understanding the high-pressure behaviors of diatomic molecules (H2, O2, N2, etc) is one of the most basic as well as important objective in high-pressure physics. Under high pressure diatomic molecule solids often exhibit rich crystal polymorphs. High-pressure isostructural transitions (HPIT) in solid hydrogen and oxygen, involving considerable technical challenges, have been experimentally documented, suggesting a possible prevailing pressure-driven molecular-symmetry breaking pathway. In spite of extensive efforts, however, HPIT in nitrogen has not been observed so far. Here we present a monoclinic-to-monoclinic isostructural phase transition (λ→λ’) in solid nitrogen at approximately 50 GPa accompanied with anomalies in lattice parameter, atomic volume and Raman vibron modes. Further ab initio calculations strongly confirmed the HPIT in nitrogen, showing the weak distortion of orientation and slight rotation in nitrogen molecules possibly drive the low-pressure phase, λ-N2, to an isostructural high-pressure phase, λ’-N2 without changing crystal symmetry. In addition, we probed in detail the phase stability and revisited the pressure-temperature (P-T) phase diagram of nitrogen, discovering a new high-pressure amorphous phase, η’-N2.