In-Plane Optical Anisotropy and Linear Dichroism in Low-Symmetry Layered TlSe

In-plane anisotropy of layered materials adds another dimension to their applications, opening up avenues in diverse angle-resolved devices. However, to fulfill a strong inherent in-plane anisotropy in layered materials still poses a significant challenge, as it often requires a low-symmetry nature of layered materials. Here, we report the fabrication of a member of layered semiconducting A^IIIB^VI compounds, TlSe, that possesses a low-symmetry tetragonal structure and investigate its anisotropic light–matter interactions. We first identify the in-plane Raman intensity anisotropy of thin-layer TlSe, offering unambiguous evidence that the anisotropy is sensitive to crystalline orientation. Further <i>in-situ</i> azimuth-dependent reflectance difference microscopy enables the direct evaluation of in-plane optical anisotropy of layered TlSe, and we demonstrate that the TlSe shows a linear dichroism under polarized absorption spectra arising from an in-plane anisotropic optical property. As a direct result of the linear dichroism, we successfully fabricate TlSe devices for polarization-sensitive photodetection. The discovery of layered TlSe with a strong in-plane anisotropy not only facilitates its applications in linear dichroic photodetection but opens up more possibilities for other functional device applications