Reconfiguring the Optical Selection Rule in Ultramicrotome‐Crafted Vertically Aligned InSe Ribbons

Abstract Due to the high carrier mobility and direct bandgap character, indium selenide (InSe) exhibits great advantages for advanced optoelectronic applications. However, the unique optical section rule in InSe weakens the light‐matter interaction when the electric field of illuminated light is perpendicular to the c‐axis of planar InSe flake. To overcome this constraint, ultramicrotome technique is introduced to achieve vertically aligned InSe ribbons, aiming to reconfigure the optical paths for improved optical absorption and device performance. The well‐designed InSe ribbons are acquired with uniform morphology, showing an integrated structure free of cracks or fragments. First, the structural symmetry, crystal orientation, and optical anisotropy of InSe ribbon are carefully revealed by polarization‐dependent Raman spectrum, second harmonic generation (SHG), and photoluminescence measurements. Then, the back focal plane (BFP) imaging of photoluminescence distinguishes the in‐plane and out‐of‐plane dipole emission of InSe ribbons and planar InSe flakes, respectively. Notably, the ribbon exhibits new PL peaks with energy lower than the exciton peak of InSe at low temperature, which is attributed to Se vacancies. The work by introducing vertically aligned InSe nanoribbons provides a new strategy to manipulate the light‐matter interactions and defect engineering for novel optoelectronics, which can be also extended to other 2D semiconductors.