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Large-area single-crystal monolayers of two-dimensional (2D) materials suchas graphene and hexagonal boron nitride (h-BN) can be grown by chemical vapourdeposition (CVD). However, the high temperatures and fast timescales at whichthe conversion from a gas-phase precursor to the 2D material appear, make itextremely challenging to simultaneously follow the atomic arrangements. Weutilise helium atom scattering to discover and control the growth of novel 2Dh-BN nanoporous phases during the CVD process. We find that prior to theformation of h-BN from the gas-phase precursor, a metastable $(3\times3)$structure is formed, and that excess deposition on the resulting 2D h-BN leadsto the emergence of a $(3\times4)$ structure. We illustrate that thesenanoporous structures are produced by partial dehydrogenation andpolymerisation of the borazine precursor upon adsorption. These steps arelargely unexplored during the synthesis of 2D materials and we unveil the richphases during CVD growth. Our results provide significant foundations for 2Dmaterials engineering in CVD, by adjusting or carefully controlling the growthconditions and thus exploiting these intermediate structures for the synthesisof covalent self-assembled 2D networks.

nanoscale horizons

Evolution of ordered nanoporous phases during h-BN growth: Controlling  the route from gas-phase precursor to 2D material by $\textit{in-situ}$  monitoring