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The two-dimensional (2D) semiconductor indium selenide (InSe) has attractedsignificant interest due its unique electronic band structure, high electronmobility and wide tunability of its band gap energy achieved by varying thelayer thickness. All these features make 2D InSe a potential candidate foradvanced electronic and optoelectronic applications. Here, we report on thediscovery of new polymorphs of InSe with enhanced electronic properties. Usinga global structure search that combines artificial swarm intelligence withfirst-principles energetic calculations, we identify polymorphs that consist ofa centrosymmetric monolayer belonging to the point group D$_{3d}$, distinctfrom the well-known polymorphs based on the D$_{3h}$ monolayers that lackinversion symmetry. The new polymorphs are thermodynamically and kineticallystable, and exhibit a wider optical spectral response and larger electronmobilities compared to the known polymorphs. We discuss opportunities tosynthesize these newly discovered polymorphs and viable routes to identify themby X-ray diffraction, Raman spectroscopy and second harmonic generationexperiments.

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