| Summary: | Consecutively tailoring few‐layer transition metal dichalcogenides MX2 from 2H to T d phase may realize the long‐sought topological superconductivity in a single material system by incorporating superconductivity and the quantum spin Hall effect together. Here, this study demonstrates that a consecutive structural phase transition from T d to 1T ′ to 2H polytype can be realized by increasing the Se concentration in Se‐substituted MoTe2 thin films. More importantly, the Se‐substitution is found to dramatically enhance the superconductivity of the MoTe2 thin film, which is interpreted as the introduction of two‐band superconductivity. The chemical‐constituent‐induced phase transition offers a new strategy to study the s+− superconductivity and the possible topological superconductivity, as well as to develop phase‐sensitive devices based on MX2 materials.
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