Metal-organic frameworks (MOFs) have emerged as a versatile class of materials. Understanding the structural and chemical properties of MOFs is essential for tailoring their performance to suit specific applications. In recent years, Raman spectroscopy, a non-destructive vibrational spectroscopic technique, has evolved into a powerful tool for characterizing MOFs. Beyond spontaneous Raman scattering, numerous advanced Raman techniques have been developed to amplify the inherently weak Raman signal. These innovations have significantly enhanced the spatial resolution, frame rate, and sensitivity of Raman imaging, thereby opening up new possibilities for applications, such as label-free sensing. This tutorial work is designed to demystify the fundamental theory and instrumentation of Raman spectroscopy, elucidating the differences between commonly used Raman techniques. Particular emphasis is placed on their advantages and limitations when applied to MOF materials. Furthermore, this work showcases how Raman techniques are employed in studying MOF systems to address societal needs and explore future directions. Ultimately, this review emphasizes the crucial role of Raman spectroscopy and the development of novel Raman-based in situ techniques to conquer the field of MOFs.

Raman scattering, celebrated for its label-free vibrational contrast, serves as an ideal means for exploring metal-organic frameworks (MOFs) through spectroscopic methods. Going beyond conventional spectroscopy, advanced Raman techniques empower in situ and in operando measurements with remarkable spatiotemporal precision. This tutorial work encompasses fundamental theory, instrumentation, and distinctions among Raman techniques, shedding light on their transformative role in probing MOFs and tackling pressing societal challenges.image