Abstract
Polarization and azimuthal dependencies of optical second-harmonic generation at the surface of cubic ionic crystals have been measured on polished surfaces of BaF2 (111) and (100), CaF2 (111) and NaCl (111), using a fundamental wavelength of 532 nm. The results are interpreted in terms of available theory, which shows that for transparent cubic media only the dipolar surface contribution depends on the crystal orientation. For BaF2 (111) and NaCl (111) the crystallineC 3vgeometry could be identified but not for CaF2 (111). Although the nature of the electronic surface structure giving rise to a dipolar polarizability remains undetermined, the experimental result suggests that it may be due to impurity or defect states in the band gap at the surface.
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This is strictly valid only for plane waves. The field gradient due to a realistic Gaussian beam profile should be negligibly small compared to\(\partial \tilde E_z /\partial z|_{z = 0} \) and only lead to a negligible, isotropic contribution to the polarization. Also, a transversal field gradient due to absorption by electronic surface states or by defect states in the bulk should be negligible compared to the respective dipole contributions, even though anisotropic
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It was pointed out in Sect. 2 that the assumption of such a term merely on the basis of symmetry arguments [26] is not justified. This is supported by the experimental observation
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Reif, J., Tepper, P., Matthias, E. et al. Surface structure of cubic ionic crystals studied by optical second-harmonic generation. Appl. Phys. B 46, 131–138 (1988). https://doi.org/10.1007/BF00686465
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DOI: https://doi.org/10.1007/BF00686465