Coherent Raman scattering spectroscopy provides a unique label-free, non-invasive approach for in situ interrogation of molecular-level information of specimen in a wide range of fields. However, it is often neglected that vibration is dynamic. Vibrational dephasing is susceptible to the nanoenvironment, and can be used as a unique probe for sensing complex intra- and inter-molecular interactions, especially in complex systems such as a living cell. By using a high dynamic range detection in time-resolved coherent Raman scattering (T-CRS) spectroscopy, we demonstrate vibrational dephasing time serves as a unique probe for sensing molecular interactions, which is in close connection to the macroscopic properties of specimen. Furthermore, such unique capability is promising for imaging applications of fields including biology, chemistry, and materials science.
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