Orbital angular momentum impact on light scattering by phonons tested experimentally

Polarized Raman spectra of piezoelectric bismuth germanate single crystal were recorded using vortex light in order to verify the predicted symmetry selection rules for Raman scattering of photons with nonzero orbital angular momentum. First, the phonon spectrum is fully characterized by the infrared reflectivity and Raman scattering with ordinary light. Then, vortex light Raman spectra were compared with the ordinary ones, but no influence of the orbital momentum on the Raman spectra of Bi4Ge3O12 was observed. In particular, we experimentally negate the theoretical prediction that Raman scattering using vortex light can yield frequencies of the silent optic modes of Bi4Ge3O12. We also have not seen evidence for the predicted symmetry-lowering of the Raman scattering tensors of E modes. We propose that the orbital momentum effects are inaccessible to the ordinary Raman spectroscopy experiments because of the tiny magnitudes of typical phonon coherence lengths.