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    Theoretical analysis of hard x-ray generation by nonperturbative interaction of ultrashort light pulses with a metal
    (Melville, NY : AIP Publishing LLC, 2015) Weisshaupt, Jannick; Juvé, Vincent; Holtz, Marcel; Woerner, Michael; Elsaesser, Thomas
    The interaction of intense femtosecond pulses with metals allows for generating ultrashort hard x-rays. In contrast to plasma theories, tunneling from the target into vacuum is introduced as electron generation step, followed by vacuum acceleration in the laser field and re-entrance into the target to generate characteristic x-rays and Bremsstrahlung. For negligible space charge in vacuum, the Kα flux is proportional to the incident intensity and the wavelength squared, suggesting a strong enhancement of the x-ray flux by mid-infrared driving pulses. This prediction is in quantitative agreement with experiments on femtosecond Cu Kα generation.
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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.