Tailored Synthesis of Heterogenous 2D TMDs and Their Spectroscopic Characterization

Abstract

Two-dimensional (2D) vertical van der Waals heterostructures (vdWHs) show great potential across various applications. However, synthesizing large-scale structures poses challenges owing to the intricate growth parameters, forming unexpected hybrid film structures. Thus, precision in synthesis and thorough structural analysis are essential aspects. In this study, we successfully synthesized large-scale structured 2D transition metal dichalcogenides (TMDs) via chemical vapor deposition using metal oxide (WO3 and MoO3) thin films and a diluted H2S precursor, individual MoS2, WS2 films and various MoS2/WS2 hybrid films (Type I: MoxW1−xS2 alloy; Type II: MoS2/WS2 vdWH; Type III: MoS2 dots/WS2). Structural analyses, including optical microscopy, Raman spectroscopy, transmission electron microscopy (TEM) with energy-dispersive X-ray spectroscopy, and cross-sectional imaging revealed that the A1g and E2g modes of WS2 and MoS2 were sensitive to structural variations, enabling hybrid structure differentiation. Type II showed minimal changes in the MoS2′s A1g mode, while Types I and III exhibited a ~2.8 cm−1 blue shift. Furthermore, the A1g mode of WS2 in Type I displayed a 1.4 cm−1 red shift. These variations agreed with the TEM-observed microstructural features, demonstrating strain effects on the MoS2–WS2 interfaces. Our study provides insights into the structural features of diverse hybrid TMD materials, facilitating their differentiation through Raman spectroscopy.