Metal stamp fabrication and patterning process
First, photolithography is conducted on a polished Si wafer to pattern the mold structure, followed by the electron beam deposition (or sputtering) of a 1 μm thick SiO2 film (deposition rate ∼1 Å s−1) and lift-off in hot acetone (Supplementary Fig. 1a and Fig. 1h). Next, 50 nm thick Au film (thermal evaporation rate ∼0.5 Å s−1) is deposited (Supplementary Fig. 1b), followed by spin-coating a 10 wt % PC (Aldrich, molecular weight ∼45 000 g/mol) layer on the surface of 3D SiO2 mold with a speed of 3000 rpm for 60 s and baked at 100 °C (3 min). With the PI tape+PDMS supporting layer, Au and PC films can be peeled-off from the Si substrate and flipped onto the surface of glass+metal frame to prepare the Au-stamp (Supplementary Fig. 1c), which inherit the inverted 3D morphology of prefabricated mold. Immediately, the 3D Au stamp is then pressed onto the surface of the as-grown 2D film and is heated at 120 °C for 5 min. After separating the stamp, large-area MoS2 arrays can be observed on substrate.
For control samples with traditional RIE method, photoresist (micro resist technology, S1850) is spin-coated onto as-grown 2D film with a speed of 6000 rpm for 60 s and baked at 110 °C (3 min), followed by the photolithography is conducted to fabricated mask patterns. Next, RIE (O2) is conducted to etching the samples (power of 50W, 10s), followed by soak in hot acetone (60 °C, 1h) to remove the photoresist mask and then MoS2 arrays is obtained.
PL and Raman characterizations
The prepared samples are placed on a confocal microscope (WITEC alpha 200R) to measure Raman and PL spectra. For PL spectrum measurement, a 532 nm laser with 1800 lines mm−1 grating is used, and laser power is 0.6 mW. For Raman spectrum measurement, a 532 nm laser is used with 1 mW power and a grating level of 2400 lines mm−1.
Monolayer MoS2 FET arrays fabrication
After patterning MoS2 arrays on grown SiO2/Si substrate (dielectric/back gate), photolithography is conducted to pattern the source/drain electrodes (TuoTuo Technology (Suzhou) Co., Ltd.), followed by deposition of Bi/Au (20 nm of Bi, 50 nm of Au) using a thermal evaporation system under vacuum (pressure ∼10−7 Torr) and lift-off. For fair comparison, the original CVD MoS2 films for two patterning methods are derived from one chip, and the device fabrication and measurement parameters are kept constant.
Wafer-scale logic circuits fabrication
After patterning MoS2 arrays on grown 2-inch sapphire substrate, first photolithography is conducted to pattern the source/drain electrodes, followed by deposition of Bi/Au (20 nm of Bi, 30 nm of Au) and lift-off. Next, Atomic layer deposition (ALD) is conducted to deposit high-κ gate dielectric (20 nm Al2O3) at 150 °C using trimethyl aluminium and water as precursors. The via of the gate dielectric layer is realized by second photolithography and solution-etching of Al2O3 by NaOH. Last, third photolithography is conducted to pattern the top gate electrodes, followed by deposition of Cr/Au (2 nm of Cr, 50 nm of Au) and lift-off. The electronic measurement of wafer-scale logic gates is conducted in air using Keithley 4200A semiconductor analyzer.