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    Real-time stimulated Raman spectroscopy with a non-collinear optical parametric oscillator
    (Washington, DC : Soc., 2021) Beichert, Luise; Binhammer, Yuliya; Andrade, José R. C.; Mevert, Robin; Kniggendorf, Ann-Kathrin; Roth, Bernhard; Morgner, Uwe
    Ultrafast detection of microplastic particles is becoming a vital problem, as these particles are found in water sources worldwide. Ideally, a live analysis in flow is desirable to directly monitor the water quality for contaminations. Therefore, coherent Raman spectroscopy techniques require fast and broadband tunable lasers to address all relevant spectral regions of the investigated samples. In our work, we combine a high power non-collinear optical parametric oscillator with a real-time stimulated Raman scattering spectroscopy setup. The light source is continously tunable from 700 nm to 1030 nm in less than 10 ms, delivering an average output power of more than 500 mW with sub-ps pulses. We show the immediate observation of mixing processes and the detection of microplastic particles in water solution with a spectral window of more than 2000 cm-1.
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    Monitoring conical intersections in the ring opening of furan by attosecond stimulated X-ray Raman spectroscopy
    (Melville, NY : AIP Publishing LLC, 2015) Hua, Weijie; Oesterling, Sven; Biggs, Jason D.; Zhang, Yu; Ando, Hideo; de Vivie-Riedle, Regina; Fingerhut, Benjamin P.; Mukamel, Shaul
    Attosecond X-ray pulses are short enough to capture snapshots of molecules undergoing nonadiabatic electron and nuclear dynamics at conical intersections (CoIns). We show that a stimulated Raman probe induced by a combination of an attosecond and a femtosecond pulse has a unique temporal and spectral resolution for probing the nonadiabatic dynamics and detecting the ultrafast (∼4.5 fs) passage through a CoIn. This is demonstrated by a multiconfigurational self-consistent-field study of the dynamics and spectroscopy of the furan ring-opening reaction. Trajectories generated by surface hopping simulations were used to predict Attosecond Stimulated X-ray Raman Spectroscopy signals at reactant and product structures as well as representative snapshots along the conical intersection seam. The signals are highly sensitive to the changes in nonadiabatically coupled electronic structure and geometry.