The limited quantum yield of strained monolayer transition metal dichalcogenides grown by vapor-phase methods and during transfer-based stacking poses a fundamental challenge for their optoelectronic applications. In this work, we propose and demonstrate “disorder engineering”—the controlled introduction of compositional or interfacial disorder to tailor electron–phonon coupling—as an effective strategy to activate efficient light emission in such materials. We show that precise selenium (Se) doping (at low concentrations, e.g., <15%) in ${\mathrm{WS}}_2$ monolayers can enhance the photoluminescence (PL) intensity by an order of magnitude under strain, whereas both undoped and heavily doped samples exhibit strong PL quenching due to the direct-to-indirect bandgap transition. This optimal enhancement is attributed to doping-induced disorder, which strengthens electron-phonon interactions and enables efficient phonon-assisted recombination of momentum-dark excitons. Furthermore, in van der Waals heterostructures, interfacial coupling to an Se-doped layer can impart additional disorder and further boost the PL via proximity effects. Our findings establish entropy engineering through controlled doping as a powerful approach for unlocking high-efficiency emission in atomically thin semiconductors.

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• Doping effects
• Phonons
• 2-dimensional systems
• Disordered alloys
• Transition metal dichalcogenides
• First-principles calculations
• Photoluminescence