Optical second harmonic generation studies of the nature of the oxide-covered and clean c(4 × 4) and (2 × 4) reconstructed GaAs(001) surfaces

Abstract

We report the application of the “epioptic” technique of optical second harmonic generation (SHG) to the study of surface chemical processes occurring at the technologically important (001) surfaces of the non-centrosymmetric compound semiconductor GaAs. SHG has been used to monitor the thermal removal of surface contamination from an GaAs(001) substrate mounted in a conventional molecular beam epitaxy (MBE) chamber. Rotational anisotropy plots of the reflected SH signal recorded at near-normal incidence indicate that the oxide layer is not fully disordered and possesses some structural anisotropy, i.e. some preferred net surface orientation. In addition the rotational anisotropy plots were observed to change in both intensity and apparent phase between the oxide-covered surface and the clean reconstructed surfaces. Following heating to 850 K under the background As 2 flux present in the chamber, the SH signal from the clean, reconstructed surface was approximately 5 × weaker than that observed for the contaminated surface and was subsequently found to be insensitive to the reconstruction change between the (2 × 4) and c(4 × 4) surfaces, in agreement with theoretical predictions for surfaces having 2mm and 4mm symmetry, respectively. These data are discussed in terms of the difficulties encountered when attempting to observe a surface SH response from a non-centrosymmetric substrate. The sensitivity of the technique towards the thin oxide overlayer suggests that for overlayers which are likely to possess net oriented in-plane dipoles due to the structural mismatch with the substrate, an SH response may be observed in preference to a bulk response when a normal incidence geometry is employed.