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- W2996562938 abstract "Surfaces and interfaces play important roles in many processes and reactions and are therefore intensively studied, often with the aim of obtaining molecular-level information from just the interfacial layer. Generally, only the first few molecular layers next to the interface are relevant for the surface processes. In the past decades, 2nd-order nonlinear spectroscopies including sum-frequency generation and second harmonic generation have developed into powerful tools for obtaining molecularly specific insights into the interfacial region. These approaches have contributed substantially to our understanding of a wide range of physical phenomena. However, along with their wide-ranging applications, it has been realized that the implied surface-specificity of these approaches may not always be warranted. Specifically, the bulk quadrupole contribution beyond the electric dipole-approximation for a system with a weak nonlinear interface signal, as well as the diffuse layer contribution at charged interfaces, could mask the surface information. In this perspective paper, we discuss the surface-specificity of 2nd-order nonlinear spectroscopy, especially considering these two contributions." @default.
- W2996562938 created "2019-12-26" @default.
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- W2996562938 date "2019-12-16" @default.
- W2996562938 modified "2023-10-18" @default.
- W2996562938 title "How surface-specific is 2nd-order non-linear spectroscopy?" @default.
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- W2996562938 doi "https://doi.org/10.1063/1.5129108" @default.
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