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We demonstrate and analyze a series of experiments in traditional and soft condensed matter using coherent optical spectroscopy and microscopy with ultrafast time resolution. We show the capabilities of resolving both real and imaginary parts of the third-order nonlinearity in the vicinity of Raman resonances from a medium probed within microscopic volumes with an equivalent spectral resolution of better than 0.1 cm−1. We can differentiate between vibrations of various types within unit cells of crystals, as well as perform targeted probes of areas within biological tissue. Vibrations within the TiO6 octahedron and the ones for the Ti-O-P intergroup were studied in potassium titanyl phosphate crystal to reveal a multiline structure within targeted phonon modes with closely spaced vibrations having distinctly different damping rates (~0.5 ps−1 versus ~1.1 ps−1). We also detected a 1.7–2.6 ps−1 decay of C-C stretching vibrations in fat tissue and compared that with the corresponding vibration in oil.

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This work is licensed under a Creative Commons Attribution 4.0 License.