Durandurdu, Murat2025-09-252025-09-2520250895-79591477-2299https://doi.org/10.1080/08957959.2025.2496647https://hdl.handle.net/20.500.12573/4080The high-pressure behavior of triazine-based amorphous C3N4, initially exhibiting a chemically ordered, graphite-like structure, was investigated using ab initio molecular dynamics simulations. Our study reveals a pressure-induced transition to a high-density amorphous (HDA) phase characterized by increased coordination number for carbon (3.88) and nitrogen (2.93) atoms. This transition occurs gradually over a broad pressure range, initiated by the breakdown of chemical ordering and the formation of homopolar C-C and N-N bonds, which persist in both the HDA and recovered phases. The recovered phase retains elevated coordination numbers (C: 3.25, N: 2.46) but loses its initial graphite-like topology, evolving into a three-dimensional network structure. Electronic structure analysis reveals semiconducting behavior in the HDA phase and n-type semiconductor characteristics in the recovered phase.eninfo:eu-repo/semantics/closedAccessCarbon NitrideGraphite-LikePolyamorphismAb InitioPressureArticle10.1080/08957959.2025.24966472-s2.0-105003114552