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The structure of amorphous materials has been debated since the 1930's as abinary question: amorphous materials are either Zachariasen continuous randomnetworks (Z-CRNs) or Z-CRNs containing crystallites. It was recentlydemonstrated, however, that amorphous diamond can be synthesized in eitherform. Here we address the question of the structure of single-atom-thickamorphous monolayers. We reanalyze the results of prior simulations foramorphous graphene and report kinetic Monte Carlo simulations based onalternative algorithms. We find that crystallite-containing Z-CRN is thefavored structure of elemental amorphous graphene, as recently fabricated,whereas the most likely structure of binary monolayer amorphous BN isaltogether different than either of the two long-debated options: it is acompositionally disordered "pseudo-CRN" comprising a mix of B-N andnoncanonical B-B and N-N bonds and containing "pseudocrystallites", namelyhoneycomb regions made of noncanonical hexagons. Implications for othernon-elemental 2D and bulk amorphous materials are discussed.

The structure of amorphous two-dimensional materials: Elemental monolayer amorphous carbon versus binary monolayer amorphous boron nitride