A set of experiments designed to study the anisotropic spatial dependence of second harmonic generation(SHG)from the surface of single crystal metals were presented. The anisotropic dependence of reflected SHG from Al₂O₃/Al(111)interface was studied. The isotropic dependence of the SHG signal is used to probe the structural symmetry of Al₂O₃/Al(111)interface. The SHG probe was also used to follow pulsed laser annealing(PLA)of the Al₂O₃/Al(111)interface. For peak laser powers per pulse ranging from 2×10⁶W/cm² to 9.6x10⁶W/cm²,the anisotropic dependence of the SHG signal was not found to vary from experiment to experiment. Using P-polarized pump laser light,the P-polarized SHG signal exhibits three equally spaced,equal intensity maxima during a single complete rotation of the Al₂O₃/Al(111)interface about the interface normal. When the incident P-polarized 1064 nm pump laser light possesses an incident peak power of 12×10⁶W/cm² per pulse,the Al₂O₃/Al(111)interface is damaged. After this damage is made,the interface does not exhibit a symmetrical anisotropic dependence in the SHG signal. Annealing of the interface is found to occur when the incident P-polarized 1064 nm pump laser light has an incident peak power of 11×10⁶W/cm² per pulse. The intensity of the P-polarized 532 nm SHG signal generated in reflection from this annealed interface exhibits a reduced anisotropic component in the SHG signal.