Lengenbachite is a naturally occurring layered mineral formed with alternating stacks of two constituent PbS-like and M2S3-like two-dimensional (2D) material layers due to the phase segregation process during the formation. Here, we demonstrate to achieve van der Waals (vdW) heterostructures of lengenbachite down to a few layer-pair thickness by mechanical exfoliation of bulk lengenbachite mineral. The incommensurability between the constituent isotropic 2D material layers makes the formed vdW heterostructure exhibit strong in-plane structural anisotropy, which leads to highly anisotropic optical responses in lengenbachite thin flakes, including anisotropic Raman scattering, linear dichroism, and anisotropic third-harmonic generation. Moreover, we exploit the nonlinear optical anisotropy for polarization-dependent intensity modulation of the converted third-harmonic optical vortices. Our study establishes lengenbachite as a new natural vdW heterostructure-based 2D material with unique optical properties for realizing anisotropic optical devices for photonic integrated circuits and optical information processing.
Exploiting polaritons in natural vdW materials has been successful in achieving extreme light confinement and low-loss optical devices and enabling simplified device integration. Recently, α-MoO3has been reported as a semiconducting biaxial vdW material capable of sustaining naturally orthogonal in-plane phonon polariton modes in IR. In this study, we investigate the polarization-dependent optical characteristics of cavities formed using α-MoO3to extend the degrees of freedom in the design of IR photonic components exploiting the in-plane anisotropy of this material. Polarization-dependent absorption over 80% in a multilayer Fabry-Perot structure with α-MoO3is reported without the need for nanoscale fabrication on the α-MoO3. We observe coupling between the α-MoO3optical phonons and the Fabry-Perot cavity resonances. Using cross-polarized reflectance spectroscopy we show that the strong birefringence results in 15% of the total power converted into the orthogonal polarization with respect to incident wave. These findings can open new avenues in the quest for polarization filters and low-loss, integrated planar IR photonics and in dictating polarization control.
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- Nature Communications
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- National Science Foundation
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Naturally occurring van der Waals heterostructure lengenbachite with strong in-plane structural and optical anisotropy
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