Tunable Optical Activity in Twisted Anisotropic Two-Dimensional Materials

Twisted van der Waals structures exhibit a variety of unusual electrical and optical phenomena and could provide a powerful means for designing nanodevices with tunable chiral properties. However, programming intrinsic chiral properties of the film on the atomic scale remains a great challenge due to the limitations of fabrication and measurement techniques. Here, we report a highly tunable large optical activity of twisted anisotropic two-dimensional (2D) materials, including black phosphorus (BP), ReS₂, PdSe₂, and α-MoO₃, by varying the twist angle between the stacked layers. The chirality can be deliberately tailored through the engineering of the symmetry, band structure, and anisotropy of 2D materials, demonstrating the high tunability of the chirality. The results show the highest thickness-normalized ellipticity value (13.8 deg μm^-1, twisted ReS₂) and ellipticity value (1581 mdeg, twisted BP) among the systems based on 2D materials. It is also shown that the chiroptical response exists in an extremely large spectral range from the visible to the infrared. Furthermore, the twisted ReS₂ enabled spin-selective control of the information transformation. These results show that highly controllable chirality in twisted 2D anisotropic materials has considerable potential in on-chip polarization optics, nano-optoelectronics, and biology.