1. How surface-specific is 2nd-order non-linear spectroscopy?
- Author
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Sun, Shumei, Schaefer, Jan, Backus, Ellen H. G., and Bonn, Mischa
- Subjects
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SECOND harmonic generation , *SPECTRUM analysis , *NONLINEAR optical spectroscopy , *PHENOMENOLOGICAL theory (Physics) , *NONLINEAR systems , *HARMONIC generation - 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. [ABSTRACT FROM AUTHOR]
- Published
- 2019
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