“…It has been suggested recently that bond hyperpolarizability models of optical second harmonic generation (SHG) [1][2][3] may be simplified by assuming that the dipolar SH radiation originates from the anharmonic motion of bond charges strictly along bond directions [4]. This assumption of a single axial component in the simplified bond hyperpolarizability model (SBHM) would allow simple interpretation of rotational SHG plots in terms of the contribution from the small number of different bonds at the surface or interface.…”
The optical second-harmonic response of native-oxide-covered vicinal Si(111), offcut by 3° towards [1 12] , is compared with previous work at the same wavelength on similar samples, but offcut by 5° in the opposite, [112] , direction. Sample rotation plots for sS, pS, sP and pP polarisation combinations are reported using 130 fs laser pulses of 765 nm wavelength, where mN indicates m-polarised input and N-polarised SH output. The two offcuts have different step geometries, but the same terrace structure at the Si/SiO 2 interface. In addition, the bulk quadrupolar contributions from the two offcuts are related by simple geometric factors. By using these constraints, simultaneous fitting of eight rotation plots allows the bulk and interface contributions to be estimated. These results offer the possibility of more detailed investigation of bond hyperpolarisability models, which have been applied recently to the vicinal Si/SiO 2 interface.
“…It has been suggested recently that bond hyperpolarizability models of optical second harmonic generation (SHG) [1][2][3] may be simplified by assuming that the dipolar SH radiation originates from the anharmonic motion of bond charges strictly along bond directions [4]. This assumption of a single axial component in the simplified bond hyperpolarizability model (SBHM) would allow simple interpretation of rotational SHG plots in terms of the contribution from the small number of different bonds at the surface or interface.…”
The optical second-harmonic response of native-oxide-covered vicinal Si(111), offcut by 3° towards [1 12] , is compared with previous work at the same wavelength on similar samples, but offcut by 5° in the opposite, [112] , direction. Sample rotation plots for sS, pS, sP and pP polarisation combinations are reported using 130 fs laser pulses of 765 nm wavelength, where mN indicates m-polarised input and N-polarised SH output. The two offcuts have different step geometries, but the same terrace structure at the Si/SiO 2 interface. In addition, the bulk quadrupolar contributions from the two offcuts are related by simple geometric factors. By using these constraints, simultaneous fitting of eight rotation plots allows the bulk and interface contributions to be estimated. These results offer the possibility of more detailed investigation of bond hyperpolarisability models, which have been applied recently to the vicinal Si/SiO 2 interface.
“…McGilp [31,32] and Arzate and Mendoza [21] note that local-field effects may be relevant in surface regions. However, the model they employ uses induced dipoles rather than bond charges, and is beyond the scope of our present discussion.…”
mentioning
confidence: 97%
“…A third advantage of bond models in general is that they provide a convenient point of contact between theory and experiment. As Levine [15] has shown in the static limit and others more generally [19][20][21], with an appropriate model the hyperpolarizabilities can be calculated and tensor coefficients evaluated.…”
mentioning
confidence: 99%
“…They found that the main contributions again came from charge displacements along the bond axes, although perpendicular components dominated for bonds that are severely bent. In the 1990s and early 2000s, Mendoza and Mochán [20] and Arzata and Mendoza [21] used an interacting-dipole model to investigate SHG arising from surface local-field effects.…”
Atomic-scale descriptions of linear-optical properties such as reflection are nearly a century old, but surprisingly, analogous models describing nonlinear-optical (NLO) properties as the natural dynamic response of bond charges driven by an external field are a recent development. These bond-charge models have proven to be particularly useful in describing the relevant physics of second-, third-, and fourth-harmonic generation, identifying previously unrecognized contributions to NLO responses, and uncovering well-disguised correlations in tensor parameters determined phenomenologically from symmetry conditions. Current capabilities are discussed, and opportunities for improved understanding noted. 1 Introduction The availability of continuum sources of radiation covering wide spectral ranges has not only made linear-optical spectroscopy possible, but also linear-optical techniques indispensable for determining information nondestructively about materials, interfaces, and structures. Owing to the higher-order tensors involved, in principle nonlinear-optical (NLO) probes are much more powerful, but spectroscopic data [1-5] have been difficult to acquire. However, commercial femtosecond systems that can tune over wide wavelength ranges are becoming available, and we are rapidly reaching the point where NLO spectroscopy will be routine.The potentially greater diagnostic power of NLO comes at a price, specifically the need to use more complex models and methods to interpret these more complex data. For most linear-optical applications, measurements can be analyzed using macroscopic parameters such as the dielectric function e, which for isotropic materials is a scalar and anisotropic materials a second-rank tensor. Here a return to fundamentals is generally unnecessary, and the last contact most linear-optical spectroscopists have had with atomic scale properties is the textbook derivation of the ClausiusMossotti relation [6], which relates the dielectric constant to local polarizabilities in the static limit.For NLO, quantities equivalent to e are the susceptibility tensors x ijk , x ijkl , etc. [7]. Symmetry-allowed NLO tensor components have been determined for all crystal classes, and
“…There are several theoretical formalisms that describe the SHG process for surfaces with different approximations and varying levels of difficulty [9,[13][14][15][16][17][18][19]. In this paper, we focus on a recent approach developed by us in Ref.…”
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.
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