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We show that the anisotropies of second-harmonic-generation (SHG) intensities of singular and vicinal (111) and (001)Si–dielectric interfaces can be described accurately as dipole radiation originating from the anharmonic motion of bond charges parallel to the bond directions. This simplified bond-hyperpolarizability model not only provides a simpler and mathematically more efficient representation of SHG, but also allows a direct physical interpretation at the bond level, which was lacking in previous approaches. Application to oxidized and nitrided Si–SiO2 interfaces provides new insight into bonding that occurs at these interfaces as well as the origin of SHG.

Simplified bond-hyperpolarizability model of second harmonic generation: Application to Si-dielectric interfaces