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Twisted multilayers of two-dimensional materials attract widespread research interest due to their intriguing electronic and optical properties related to their chiral symmetry breaking and moiré effects. The two-dimensional transition metal dichalcogenide MoSe2 is a particularly promising material for twisted multilayers, capable of sustaining moiré excitons. Here, we report on a rational bottom-up synthesis approach for twisted MoSe2 flakes by chemical vapor transport (CVT). Screw dislocation-driven growth was forced by surface-fused SiO2 nanoparticles on the substrates that serve as potential nucleation points in low supersaturation condition. Thus, crystal growth by in-situ CVT under addition of MoCl5 leads to bulk 2H-MoSe2 in a temperature gradient from 900 to 820 °C with a dwell time of 96 h. Hexagonally shaped 2H-MoSe2 flakes were grown from 710 to 685 °C with a dwell time of 30 min on SiO2@Al2O3(0001) substrates. Electron backscatter diffraction as well as electron microscopy reveals the screw dislocation-driven growth of triangular 3R-MoSe2 with individual step heights between 0.9 and 2.9 nm on SiO2@Si(100) under the same conditions. Finally, twisted MoSe2 flakes exhibiting a twist angle of 19° with respect to the [010] zone axis could be synthesized.

This is an open access article under the terms of the Creative Commons Attribution 4.0 International License (CC BY 4.0, https://creativecommons.org/licenses/by/4.0/).
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