We recently discovered a novel ultrafast coupling mechanism of femtosecond solitons via coherent optical phonons inside a solid-state laser cavity, forming stably bound states - “Soliton molecules”[1]. Moreover, preceding the stable binding, the relative motion of two solitons can be harnessed to sample THz phonons using real-time spectroscopy within a single rapid all-optical delay sweep. In this contribution, we discuss the sampling and contrast mechanism for highspeed spectroscopy and compare the scheme to conventional extra-cavity time-domain Raman sampling schemes. [1] A. Völkel et al., Intracavity Raman Scattering couples Soliton Molecules with Terahertz Phonons, Nature Comms. 13 (1) (2022)

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Georg Herink, Alexandra Völkel, and Timo Wirth, "Stimulated time-domain raman spectroscopy inside a femtosecond laser cavity," Proc. SPIE PC12406, Real-time Measurements, Rogue Phenomena, and Single-Shot Applications VIII, PC124060A (Presented at SPIE LASE: February 01, 2023; Published: 17 March 2023); https://doi.org/10.1117/12.2656637.6321499390112.