Gruber, ChristophChristophGruberPupeikis, JustinasJustinasPupeikisCamenzind, Sandro L.Sandro L.CamenzindWillenberg, BenjaminBenjaminWillenbergCamargo, Franco V. A.Franco V. A.CamargoLang, LukasLukasLangHamm, PeterPeterHammRampur, AnupamaaAnupamaaRampurHeidt, AlexanderAlexanderHeidtPhillips, Christopher R.Christopher R.PhillipsCerullo, GiulioGiulioCerulloKeller, UrsulaUrsulaKeller2025-03-262025-03-262024-11-06https://boris-portal.unibe.ch/handle/20.500.12422/207653Amplifier-based pump-probe systems, while versatile, often suffer from complexity and low measurement speeds, especially when probing samples require low excitation fluences. To address these limitations, we introduce a pump-probe system that leverages a 60-MHz single-cavity dual-comb oscillator and an ultra-low noise supercontinuum. The setup can operate in equivalent time sampling or in programmable optical delay generation modes. We employ this system to study the wavelength-dependent excited-state dynamics of the non-fullerene electron acceptor Y6, a compound of interest in solar cell development, with excitation fluences as low as 1 nJ/cm<jats:sup>2</jats:sup>, well below the onset of nonlinear exciton annihilation effects. Our measurements reach a shot-noise limited sensitivity in differential transmission of 3.4·10<jats:sup>–7</jats:sup>. The results demonstrate the system’s potential to advance the field of ultrafast spectroscopy.</jats:p>enarticle10.48620/865523954669210.1364/OL.538105