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Nearly two-dimensional diamond, or diamane, is coveted as ultrathin$sp^3$-carbon film with unique mechanics and electro-optics. The very thinness($~h$) makes it possible for the surface chemistry, e.g. adsorbed atoms, toshift the bulk phase thermodynamics in favor of diamond, from multilayergraphene. Thermodynamic theory coupled with atomistic first principlescomputations predicts not only the reduction of required pressure($p/p_{\infty}>1-h_0/h$), but also the nucleation barriers, definitive for thekinetic feasibility of diamane formation. Moreover, the optimal adsorbentchair-pattern on a bilayer graphene results in a cubic diamond lattice, whilefor thicker precursors the adsorbent boat-structure tends to produce hexagonaldiamond (lonsdaleite), if graphene was in AA` stacking to start with. Asadsorbents, H and F are conducive to diamond formation, while Cl appearssterically hindered.

Nano-thermodynamics of chemically induced graphene-diamond transformation