Theoretical study of electronic sum frequency generation spectroscopy to assess the buried interfaces

Abstract

This article provides a comprehensive theoretical background of electronic sum frequency generation (ESFG), a second-order nonlinear spectroscopy technique. ESFG is utilized to investigate both exposed and buried interfaces, which are challenging to study using conventional spectroscopic methods. By overlapping two incident beams at the interface, ESFG generates a beam at the sum of their frequencies, allowing for the extraction of valuable interfacial molecular information such as molecular orientation and density of states present at interfaces. The unique surface selectivity of ESFG arises from the absence of inversion symmetry at the interfaces. However, detecting weak signals from interfaces requires the ultrafast lasers to generate a sufficiently strong signal. By understanding the theoretical foundations of ESFG presented in this article, readers can gain a solid grasp of the basics of ESFG spectroscopy.