Evolution of Electronic Structure in Weyl Semimetal Mo _<i>x</i> W _1‐ _<i>x</i> Te ₂

Mo x W 1‐ x Te 2 Weyl semimetal has emerged as a promising candidate for realizing tunable Fermi arc surface states, with potential applications in spintronics and topological quantum materials. Compositions in the range x = 0.1 to 0.5 crystallize in a mixed phase comprising noncentrosymmetric orthorhombic ( T d ) and centrosymmetric (1T′) structures. In this study, the surface and electronic structures of Mo x W 1‐ x Te 2 ( x = 0.1, 0.3, and 0.5) is explored using low‐energy electron diffraction (LEED), X‐ray photoelectron spectroscopy (XPS), and angle‐resolved photoemission spectroscopy (ARPES). LEED patterns exhibit sharper features for x = 0.3, suggesting enhanced crystallinity and reduced lattice distortion, attributed to stabilization of the T d phase. XPS analysis reveals asymmetric charge transfer between Te–Mo and Te–W bonding environments across all compositions, with the most pronounced modifications at x = 0.3. ARPES measurements confirm the presence of Fermi arc surface states uniquely in the x = 0.3 sample, consistent with the emergence of a type‐II Weyl semimetal phase. In contrast, increased disorder and dominance of the 1T′ phase in x = 0.5 obscure topological signatures. These results underscore the crucial role of compositional tuning in modulating structural and electronic properties, offering new insights into the design of topological phases in transition metal dichalcogenides.