Abstract
This study presents a novel strategy for controlling the orientation of MoS(2) films on thick metallic substrates through precise regulation of the sulfur flux alone. In contrast to previous approaches that rely on substrate modifications or complex parameter tuning, orientation control is achieved here solely by adjusting the sulfur concentration during the sulfurization of 400 nm RF-sputtered Mo films. The metallic Mo substrate also allows potential film transfer via selective etching-analogous to the graphene/Cu system-providing a viable route for device integration on arbitrary substrates. Analyses (XRD, Raman, and TEM) reveal that low sulfur flux (30-50 sccm) favors horizontal growth, whereas high flux (>300 sccm) induces vertical orientation. To rationalize this behavior, a reaction-diffusion model based on the Thiele modulus was developed, quantitatively linking sulfur flux to film orientation and identifying critical thresholds (~50 and ~300 sccm) governing the horizontal-to-vertical transition. This unified approach enables the realization of distinct MoS(2) orientations using identical materials and processes, analogous to the orientation control in graphene growth on copper. The ability to grow orientation-controlled MoS(2) on non-noble metal substrates opens new opportunities for integrating electronic (horizontal) and catalytic (vertical) functionalities, thereby advancing scalable manufacturing of TMDC-based technologies.