Helicity‐Dependent Raman Spectroscopy of Diamond and Zinc‐Blende Crystal Structures

ABSTRACT We calculate polarized Raman intensity of diamond and zinc‐blende crystal structure for arbitrary surfaces in a backscattering geometry using both linearly and circularly polarized light. Rotated Raman tensors are applied to the phonon mode of diamond and the (LO/TO) phonon modes of zinc blende to evaluate how the Raman intensity evolves as the surface orientation is varied from (100) toward (110) and (111). Polar plots versus sample rotation angle or analyzer angle show distinct behaviors for parallel (VV) and cross (VH) configurations under linear polarization, as well as helicity‐dependent configuration. Helicity‐dependent Raman spectroscopy reveals surface‐dependent tilts of the polar pattern. We derive the analytical expressions for the Raman intensities and for the angular positions of maxima and minima as explicit functions of . These surface orientation‐sensitive signatures enable identification of unknown , including sample miscut, and allow predictive modeling of polar‐plot evolution, improving the precision of polarized Raman surface metrology.