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Coherent anti‐Stokes Raman scattering is a powerful nonlinear optical spectroscopic technique primarily used in chemistry and biology for detection and diagnostics by excitation and probing of coherent molecular vibrations. Despite many advantages, there are certain limitations to the application of this technique due to the existence of the non‐resonant four‐wave mixing contamination. This issue is addressed here by offering the time‐resolved exact solutions with all Gaussian input pulses. The paper explains signal enhancement with a suppression of the background at the threshold delay time of the probe and presents a one‐to‐one comparison between the solutions and experimental observations that provides a reconstruction of the pure coherent Raman resonant contribution. These findings add to the deep understanding of coherent Raman spectroscopic experimental data as a hands‐on interpreting tool. Copyright © 2016 John Wiley & Sons, Ltd.

Quantitative interpretation of time‐resolved coherent anti‐Stokes Raman spectroscopy with all Gaussian pulses