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Sum-frequency generation (SFG) vibrational spectroscopy is a second-order nonlinear optical spectroscopy technique. Owing to its interfacial selectivity, SFG vibrational spectroscopy can provide interfacial molecular information, such as molecular orientations and order, which can be obtained directly, or molecular density, which can be acquired indirectly. Interfacial molecular behaviors are considered the basic factors for determining the tribological properties of surfaces. Therefore, owing to its ability to detect the molecular behavior in buried interfaces  in situ  and in real time, SFG vibrational spectroscopy has become one of the most appealing technologies for characterizing mechanisms at friction interfaces. This paper briefly introduces the development of SFG vibrational spectroscopy and the essential theoretical background, focusing on its application in friction and lubrication interfaces, including film-based, complex oil-based, and water-based lubricating systems. Real-time detection using SFG promotes the nondestructive investigation of molecular structures of friction interfaces  in situ  with submonolayer interface sensitivity, enabling the investigation of friction mechanisms. This review provides guidance on using SFG to conduct friction analysis, thereby widening the applicability of SFG vibrational spectroscopy.

Applications of sum-frequency generation vibrational spectroscopy in friction interface