“…In the first growth step, Figure a (i), 4-(4-thiophenyl)pyridine (TPP) (b), 4-(1 H -pyrrole-1-yl)thiophenol (PTP) (c), or 4-(2,5-dimethyl-1 H -pyrrole-1-yl)thiophenol (DPTP) (d) compounds form a SAM on a copper substrate by vapor deposition (VD) under vacuum. In the second step, Figure a (ii), low-energy electron irradiation induced cross-linking converts the SAM into a molecular nanosheet: a carbon nanomembrane (CNM). − CNMs have been fabricated from different molecules, and their structure and mechanical, optical, and electrical behavior can be engineered in this way. − The vacuum pyrolysis results in their conversion into graphene. ,− For the N-containing molecules (TPP, PTP, DPTP, Figure b) investigated in this study, we show that for a low pyrolysis temperature T p 1 nitrogen-doped nanocrystalline graphene is formed, Figure a (iii). By increasing the temperature to T p 2 , the recrystallization of the graphene sheet leads to the formation of nanopores by extrusion of the nitrogen atoms, Figure a (iv).…”