Improved ab initio calculation of surface second-harmonic generation from Si(111)(1×1):H

We carry out an improved ab initio calculation of surface second-harmonic generation (SSHG) from the Si(111)(1×1):H surface. This calculation includes three new features in one formulation: (i) the scissors correction, (ii) the contribution of the nonlocal part of the pseudopotentials, and (iii) the inclusion of a cut function to extract the surface response, all within the independent particle approximation. We apply these improvements on the Si(111)(1×1):H surface and compare with various experimental spectra from several different sources. We also revisit the three-layer model for the SSHG yield and demonstrate that it provides more accurate results over several, more common, two-layer models. We demonstrate the importance of using properly relaxed coordinates for the theoretical calculations. We conclude that this approach to the calculation of the second-harmonic spectra is versatile and accurate within this level of approximation. This well-characterized surface offers an excellent platform for comparison with theory and allows us to offer this study as an efficient benchmark for this type of calculation.