Surface second harmonic generation is a method for probing interfaces in atomic and molecular systems. In second harmonic generation (SHG), the light frequency is doubled, essentially converting two photons of the original beam of energy E into a single photon of energy 2E as it interacts with noncentrosymmetric media. Surface second harmonic generation is a special case of SHG where the second beam is generated because of a break of symmetry caused by an interface. Since centrosymmetric symmetry in centrosymmetric media is only disrupted in the first (occasionally second and third) atomic or molecular layer of a system, properties of the second harmonic signal then provide information about the surface atomic or molecular layers only. Surface SHG is possible even for materials which do not exhibit SHG in the bulk.[1] Although in many situations the dominant second harmonic signal arises from the broken symmetry at the surface, the signal in fact always has contributions from both the surface and bulk.[2] Thus, the most sensitive experiments typically involve modification of a surface and study of the subsequent modification of the harmonic generation properties.