Elastic Properties and Deformation Mechanisms in the van der Waals Single‐Crystalline Indium Selenide

Abstract

The bulk van der Waals (vdW) single‐crystalline indium selenide (β‐InSe) displays exceptional plasticity in a layered crystalline form at both micro‐ and macroscale. However, the nanoscale origin of plasticity remains unclear. Herein, an atomic‐level study on the deformation mechanisms of InSe by using first‐principles calculations is reported. Remarkable anisotropic elasticity is observed in the vdW InSe layered crystal, and the stiffness is dramatically softened because of the vdW gap in the layered structure. The simulations capture the distinct fracture modes in the uniaxial tensile deformation, depending on the loading directions—brittle fracture in the [100] and [110] directions while ductile failure in the [001] direction. The InSe layered crystal structure exhibits superplastic deformability under uniaxial compression. Different transition pathways, including interlayer tangling, amorphization, and cross‐linking, are tracked along respective deformation directions. The unprecedented plasticity of InSe layered crystals can be attributed to the phase transition coupled with interlayer gliding and cross‐layer dislocation slipping. This study deepens our understanding of the deformation mechanisms of layered materials at the atomistic level and provides insights into tailoring material properties for low‐dimensional material design based on its deformation mechanisms.