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Abstract 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.
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This content will become publicly available on April 1, 2026
Anisotropic Third‐Harmonic Vortex Beam Generation with Ultrathin Germanium Arsenide Fork Gratings
Abstract Optical vortices have the tremendous potential to increase data capacity by leveraging the extra degree of freedom of orbital angular momentum. On the other hand, anisotropic 2D materials are promising building blocks for future integrated polarization‐sensitive photonic and optoelectronic devices. Here, highly anisotropic third‐harmonic optical vortex beam generation is demonstrated with fork holograms patterned on ultrathin 2D germanium arsenide flakes. It is shown that the anisotropic nonlinear vortex beam generation can be achieved independent of the fork grating orientation with respect to the crystallographic orientation. Furthermore, 2D fork hologram is designed to generate multiple optical vortices having different topological charges with strong anisotropic responses. These results pave the way toward the advancement of 2D material‐based anisotropic nonlinear optical devices for future applications in photonic integrated circuits, optical communication, and optical information processing.
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- PAR ID:
- 10612023
- Publisher / Repository:
- Wiley-VCH
- Date Published:
- Journal Name:
- Laser & Photonics Reviews
- Volume:
- 19
- Issue:
- 7
- ISSN:
- 1863-8880
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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