Vibrational Sum-Frequency Generation Hyperspectral Microscopy for Molecular Self-Assembled Systems

In this review, we discuss the recent developments and applications of vibrational sum-frequency generation (VSFG) microscopy. This hyperspectral imaging technique can resolve systems without inversion symmetry, such as surfaces, interfaces and noncentrosymmetric self-assembled materials, in the spatial, temporal, and spectral domains. We discuss two common VSFGmicroscopy geometries: wide-field and confocal point-scanning. We then introduce the principle of VSFG and the relationships between hyperspectral imaging with traditional spectroscopy, microscopy, and time-resolved measurements. We further highlight crucial applications of VSFG microscopy in self-assembledmonolayers, cellulose in plants, collagen fibers, and lattice self-assembled biomimetic materials. In these systems, VSFGmicroscopy reveals relationships between physical properties that would otherwise be hidden without being spectrally, spatially, and temporally resolved. Lastly, we discuss the recent development of ultrafast transient VSFG microscopy, which can spatially measure the ultrafast vibrational dynamics of self-assembled materials. The review ends with an outlook on the technical challenges of and scientific potential for VSFG microscopy.

Automated summary

This review discusses the recent developments and applications of vibrational sum-frequency generation (VSFG) microscopy, highlighting its relationship with traditional spectroscopy, microscopy, and time-resolved measurements. Crucial applications of VSFG microscopy in self-assembled materials were emphasized, revealing hidden relationships between physical properties. The review also touches upon the recent development of ultrafast transient VSFG microscopy, offering spatial measurements of the ultrafast vibrational dynamics of self-assembled materials.