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We study the bulk contribution to surface second-harmonic generation. It is shown that the formalism in the earlier literature neglected an important term in the bulk contribution which makes the separation of surface and bulk contributions impossible in experiments that allow no modification of the sample. Isotropic and cubic systems media are discussed in some detail for illustration. We also present a model for the bulk nonlinearity of molecular systems.
Guyot‐Sionnest et al. (Sat,) studied this question.