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The crystallographic orientation of anisotropic 2D materials plays a crucial role in their physical properties and device performance. However, standard orientation techniques such as transmission electron microscopy (TEM) or X‐ray diffraction can be complex and less accessible for routine characterization. Herein, the orientation of black phosphorus (BP) from bulk crystals to thin layers is investigated using angle‐resolved polarized Raman spectroscopy with a single‐wavelength (514 nm) Raman setup. By incorporating thickness‐dependent interference effects and anisotropic optical indices, this approach provides a reliable framework for orientation determination across different BP thicknesses. The method is validated through direct orientation measurements using TEM and electron backscattering diffraction, confirming its applicability to both thick and ultrathin samples. Given its simplicity and compatibility with widely available Raman setups, this approach offers a practical solution for characterizing BP orientation without requiring advanced structural characterization techniques.
Carré et al. (Mon,) studied this question.