Abstract
Second-order optical nonlinear spectroscopy such as Second Harmonic Generation (SHG) is inherently sensitive to interfacial regions. Using our recently developed method of Interference SHG Anisotropy (ISHGA), the anisotropy of the SHG field E(2ω, ϕ)∝ ∑ mn=0 k n cos[n (ϕ+ζn)] = A+B cos(ϕ+α)+... can be measured (i.e., the variation of the 2ω-field generated during the rotation of the sample around the surface normal). This field can be separated into its various sources, denoted as A, B,..., permitting us to achieve information on the geometric and electronic structure of the interface and their changes upon potential and adsorption.
In this chapter we report on halide ion adsorption at Au(111) electrodes employing the ISHGA technique. The results show that even the isotropic contribution to SHG encodes a remarkable dependence on the various adlayer structures such as the formation of disordered, ordered and compressed adlayers in the case of specific adsorption. This contrasts with earlier assumptions that the isotropic part of the EM field (the A term) should be insensitive to structural changes of surface. Evidently, the isotropic property refers to its insensitivity with respect to the azimuthal rotation of the sample. But this does not rule out the possibility that the magnitude and complex phase of the A term depend on the interfacial structure and composition.
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Pettinger, B., Bilger, C., Lipkowski, J. (2003). SHG Studies on Halide Adsorption at Au(111) Electrodes. In: Wandelt, K., Thurgate, S. (eds) Solid—Liquid Interfaces. Topics in Applied Physics, vol 85. Springer, Berlin, Heidelberg. https://doi.org/10.1007/3-540-44817-9_7
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