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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.
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    Phonon anharmonicities and ultrafast dynamics in epitaxial Sb2Te3
    ([London] : Macmillan Publishers Limited, part of Springer Nature, 2020) Bragaglia, V.; Ramsteiner, M.; Schick, D.; Boschker, J.E.; Mitzner, R.; Calarco, R.; Holldack, K.
    In this study we report on the investigation of epitaxially grown Sb2Te3 by employing Fourier-Transform transmission Spectroscopy (FTS) with laser-induced Coherent Synchrotron Radiation (CSR) in the Terahertz (THz) spectral range. Static spectra in the range between 20 and 120 cm−1 highlight a peculiar softening of an in-plane IR-active phonon mode upon temperature decrease, as opposed to all Raman active modes which instead show a hardening upon temperature decrease in the same energy range. The phonon mode softening is found to be accompanied by an increase of free carrier concentration. A strong coupling of the two systems (free carriers and phonons) is observed and further evidenced by exciting the same phonon mode at 62 cm−1 within an ultrafast pump-probe scheme employing a femtosecond laser as pump and a CSR single cycle THz pulse as probe. Separation of the free carrier contribution and the phonon resonance in the investigated THz range reveals that, both damping of the phonon mode and relaxation of hot carriers in the time domain happen on the same time scale of 5 ps. This relaxation is about a factor of 10 slower than expected from the Lorentz time-bandwidth limit. The results are discussed in the framework of phonon scattering at thermal and laser induced transient free carriers.