Quasi‐1D ZrS3 as an Anisotropic Nano‐Reflector for Manipulating Light–Matter Interactions

Abstract 2D layered materials with low crystal symmetries exhibit unique anisotropic physical properties. Here the systematic studies on the optical modulation effects of such anisotropic 2D materials to isotropic 2D materials in their stacked van der Waals (vdW) heterostructures are reported. By applying angle‐resolved polarization spectroscopic characterizations on the MoS 2 /ZrS 3 vdW heterostructure, periodic intensity variations of the Raman scattering and photoluminescence (PL) emission modes of monolayer MoS 2 are observed, which are closely correlated to the anisotropic optical properties of the underlying ZrS 3 layers. Such anisotropic optical modulation effects can be identified with the thickness of ZrS 3 reduced to few layers (≈6 nm), and are attributed to the strong birefringence and dichroism effects in ZrS 3 that cause reflection difference between its crystal axis, thus modulating the Raman/PL intensities of MoS 2 via Fabry–Pérot interference effect. Furthermore, the polarized photocurrent response of the heterostructure is also demonstrated, where its major contribution originates from MoS 2 . This work develops a new methodology to tune the light–matter interactions and properties of isotropic 2D materials by the combination with anisotropic 2D materials, which substantially broadens the application of low symmetry layered materials in polarization sensitive optoelectronic devices.