Anomalous narrow-band optical anisotropy of MoO2 crystal in the visible regime

The emergence of anisotropic two-dimensional (2D) materials provides a platform for the cutting-edge nano- and optoelectronic devices. Exploring low-dimensional materials and revealing their anisotropic behavior are crucial for designing angle-dependent nanodevices. The metallicity of molybdenum dioxide (MoO2) crystal differentiates it from the most commonly studied semi-conductive anisotropic 2D materials. However, the studies on its optical anisotropy are still lacking. Here, two most commonly obtained shapes of rhombic and hexagonal MoO2 were synthesized by one step method of chemical vapor deposition. The rhombic and hexagonal MoO2 display a slight frequency shift of 1–5 cm−1 depending on the variation modes, but the Raman modes at 366 cm−1 remain unaltered. Using a combination of differential reflectance spectroscopy and reflectance difference spectroscopy, we revealed the unusual narrow-band optical anisotropies of rhombic and hexagonal MoO2 crystals in the visible wavelength region due to its unique metallic properties. Furthermore, it is found that the center wavelengths of the narrow-band optical anisotropy of the MoO2 crystal can be effectively adjusted by coherent optical interference. Our results present an interesting anisotropic metallic 2D candidate and an effective cavity-based approach to regulate the center wavelengths of as-obtained narrow-band optical anisotropy, which is highly beneficial for the wavelength-selected devices.