Fig. 1: Building m∙2N-layer artificial crystals with exponentially growing thickness.

a The schematic concept of constructing an m∙2N-layer superlattice with N-time operation, where N represents the stacking rounds, and m denotes the layer number of the initial material unit. b The “picking-up—pressing and dividing—picking-up—restacking” procedure. c Crystal layer number (n) versus operation times (N) of this work (red symbols; the fit curve is n = 2N) and the layer-by-layer approach (gray symbols; the fit curve is n = 1 + N), for clearance, we take m = 1 as an example. d Schematic illustration of identical interlayer alignment with zero twist angle for the 2N method. Photos of a centimeter-scale MoS2 single crystal grown by chemical vapor deposition (CVD) (e), as-prepared ladder-like millimeter-scale 16 layers (16L) MoS2 crystal (f) and the corresponding schematic structure (g). Optical microscopy images of a near 0° WSe2/MoS2 heterobilayer (h), as-prepared 8L WSe2/(MoS2/WSe2)3/MoS2 heterogeneous superlattice (i) and corresponding schematic structure (j).