Excitonic Landscapes in Monolayer Lateral Heterostructures Revealed by Unsupervised Machine Learning

Abstract Two‐dimensional (2D) in‐plane heterostructures including compositionally graded alloys and lateral heterostructures with defined interfaces display rich optoelectronic properties and offer versatile platforms to explore one‐dimensional (1D) interface physics and many‐body interaction effects. Graded Mo x W 1 − x S 2 alloys show smooth spatial variations in composition and strain that continuously tune excitonic emission, while MoS 2 –WS 2 lateral heterostructures contain atomically sharp interfaces supporting 1D excitonic phenomena. These single‐layer systems combine tunable optical and electronic properties with potential for stable, high‐performance optoelectronic devices. Hyperspectral and nano‐resolved photoluminescence (PL) imaging enable spatial mapping of optical features along with local variations in composition, strain, and defects, but manual interpretation of such large datasets is slow and subjective. Here, a fast and scalable unsupervised machine‐learning (ML) framework is introduced to extract quantitative and interpretable information from hyperspectral PL datasets of graded Mo x W 1 − x S 2 alloys and MoS 2 –WS 2 heterostructures. Combining principal‐component analysis (PCA), t‐distributed stochastic neighbor embedding (t‐SNE), and density‐based spatial clustering of applications with noise (DBSCAN), spectrally distinct domains associated with composition, strain, and defect variations are uncovered. Decomposition of representative spectra reveals multiple emission species, including band‐edge excitons and defect‐related transitions, demonstrating that ML‐driven analysis provides a robust and automated route to interpret rich optical properties of 2D materials.