Maximum Achievable N Content in Atom-by-Atom Growth of Amorphous Si-B-C-N Materials

Amorphous Si-B-C-N alloys can combine exceptional oxidation resistance up to 1500 °C with high-temperature stability of superior functional properties. Because some of these characteristics require as high N content as possible, the maximum achievable N content in amorphous Si-B-C-N is examined by combining extensive ab initio molecular dynamics simulations with experimental data. The N content is limited by the formation of unbonded N2 molecules, which depends on the composition (most intensive in C rich materials, medium in B rich materials, least intensive in Si-rich materials) and on the density (increasing N2 formation with decreasing packing factor when the latter is below 0.28, at a higher slope of this increase at lower B content). The maximum content of N bonded in amorphous Si-B-C-N networks of lowest-energy densities is in the range from 34% to 57% (materials which can be grown without unbonded N2) or at most from 42% to 57% (at a cost of affecting materials characteristics by unbonded N2). The results are important for understanding the experimentally reported nitrogen contents, design of stable amorphous nitrides with optimized properties and pathways for their preparation, and identification of what is or is not possible to achieve in this field.