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New Polymorphs of Two-Dimensional Indium Selenide with Enhanced Electronic Properties

The two-dimensional (2D) semiconductor indium selenide (InSe) has attracted significant interest due its unique electronic band structure, high electron mobility and wide tunability of its band gap energy achieved by varying the layer thickness. All these features make 2D InSe a potential candidate for advanced electronic and optoelectronic applications. Here, we report on the discovery of new polymorphs of InSe with enhanced electronic properties. Using a global structure search that combines artificial swarm intelligence with first-principles energetic calculations, we identify polymorphs that consist of a centrosymmetric monolayer belonging to the point group D$_{3d}$, distinct from the well-known polymorphs based on the D$_{3h}$ monolayers that lack inversion symmetry. The new polymorphs are thermodynamically and kinetically stable, and exhibit a wider optical spectral response and larger electron mobilities compared to the known polymorphs. We discuss opportunities to synthesize these newly discovered polymorphs and viable routes to identify them by X-ray diffraction, Raman spectroscopy and second harmonic generation experiments.