Programmable Carbon Nanotube Networks: Controlling Optical Properties Through Orientation and Interaction.

The lattice geometry of natural materials and the structural geometry of artificial materials are crucial factors determining their physical properties. Most materials have predetermined geometries that lead to fixed physical characteristics. Here, the demonstration of a carbon nanotube network serves as an example of a system with controllable orientation achieving on-demand optical properties. Such a network allows programming their optical response depending on the orientation of the constituent carbon nanotubes and leads to the switching of its dielectric tensor from isotropic to anisotropic. Furthermore, it also allows for the achievement of wavelength-dispersion for their principal optical axes - a recently discovered phenomenon in van der Waals triclinic crystals. The results originate from two unique carbon nanotubes features: uniaxial anisotropy from the well-defined cylindrical geometry and the intersection interaction among individual carbon nanotubes. The findings demonstrate that shaping the relative orientations of carbon nanotubes or other quasi-one-dimensional materials of cylindrical symmetry within a network paves the way to a universal method for the creation of systems with desired optical properties.

Wandering principal optical axes in van der Waals triclinic materials.

Nature is abundant in material platforms with anisotropic permittivities arising from symmetry reduction that feature a variety of extraordinary optical effects. Principal optical axes are essential characteristics for these effects that define light-matter interaction. Their orientation - an orthogonal Cartesian basis that diagonalizes the permittivity tensor, is often assumed stationary. Here, we show that the low-symmetry triclinic crystalline structure of van der Waals rhenium disulfide and rhenium diselenide is characterized by wandering principal optical axes in the space-wavelength domain with above π/2 degree of rotation for in-plane components. In turn, this leads to wavelength-switchable propagation directions of their waveguide modes. The physical origin of wandering principal optical axes is explained using a multi-exciton phenomenological model and ab initio calculations. We envision that the wandering principal optical axes of the investigated low-symmetry triclinic van der Waals crystals offer a platform for unexplored anisotropic phenomena and nanophotonic applications.

Exploring van der Waals materials with high anisotropy: geometrical and optical approaches.

The emergence of van der Waals (vdW) materials resulted in the discovery of their high optical, mechanical, and electronic anisotropic properties, immediately enabling countless novel phenomena and applications. Such success inspired an intensive search for the highest possible anisotropic properties among vdW materials. Furthermore, the identification of the most promising among the huge family of vdW materials is a challenging quest requiring innovative approaches. Here, we suggest an easy-to-use method for such a survey based on the crystallographic geometrical perspective of vdW materials followed by their optical characterization. Using our approach, we found As2S3 as a highly anisotropic vdW material. It demonstrates high in-plane optical anisotropy that is ~20% larger than for rutile and over two times as large as calcite, high refractive index, and transparency in the visible range, overcoming the century-long record set by rutile. Given these benefits, As2S3 opens a pathway towards next-generation nanophotonics as demonstrated by an ultrathin true zero-order quarter-wave plate that combines classical and the Fabry-Pérot optical phase accumulations. Hence, our approach provides an effective and easy-to-use method to find vdW materials with the utmost anisotropic properties.