▎ 摘　　要

Nearly 2D diamond, or diamane, is coveted as an ultrathin sp(3)-carbon film with unique mechanics and electro-optics. The very thinness (approximate to h) makes it possible for the surface chemistry, for example, adsorbed atoms, to shift the bulk phase thermodynamics in favor of diamond, from multilayer graphene. Thermodynamic theory coupled with atomistic first principles computations predicts not only the reduction of required pressure (p/p(infinity) > 1 - h(0)/h) but also the nucleation barriers, definitive for the kinetic feasibility of diamane formation. Moreover, the optimal adsorbent chair-pattern on a bilayer graphene results in a cubic diamond lattice, while for thicker precursors the adsorbent boat-structure tends to produce hexagonal diamond (lonsdaleite), if graphene is in AA ' stacking to start with. As adsorbents, H and F are conducive to diamond formation, while Cl appears sterically hindered.