Attosecond Dynamics in Liquids
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2024
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Book Chapter
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Abstract
Attosecond science is well developed for atoms and promising results have been obtained for molecules and solids. Here, we review the first steps in developing attosecond time-resolved measurements in liquids. These advances provide access to time-domain studies of electronic dynamics in the natural environment of chemical reactions and biological processes. We concentrate on two techniques that are representative of the two main branches of attosecond science: pump-probe measurements using attosecond pulses and high-harmonic spectroscopy (HHS). In the first part, we discuss attosecond photoelectron spectroscopy with cylindrical microjets and its application to measure time delays between liquid and gaseous water. We present the experimental techniques, the new data-analysis methods, and the experimental results. We describe in detail the conceptual and theoretical framework required to describe attosecond chronoscopy in liquids at a quantum-mechanical level. This includes photoionization delays, scattering delays, as well as a coherent description of electron transport and (laser-assisted) photoemission and scattering. As a consequence, we show that attosecond chronoscopy of liquids is, in general, sensitive to both types of delays, as well as the electron mean-free paths. Through detailed modeling, involving state-of-the-art quantum scattering and Monte-Carlo trajectory methods, we show that the photoionization delays dominate in attosecond chronoscopy of liquid water at photon energies of 20–30 eV. This conclusion is supported by a near-quantitative agreement between experiment and theory. In the second part, we introduce HHS of liquids based on flat microjets. These results represent the first observation of high-harmonic generation (HHG) in liquids extending well beyond the visible into the extreme-ultraviolet regime. We show that the cut-off energy scales almost linearly with the peak electric field of the driver and that the yield of all harmonics scales non-perturbatively. We also discuss the ellipticity dependence of the liquid-phase harmonics, which is systematically broadened compared to the gas phase. We introduce a strongly driven few-band model as a zero-order approximation of HHG in liquids and demonstrate the sensitivity of HHG to the electronic structure of liquids. Finally, we discuss more advanced approaches for modeling liquid-phase HHG. In the conclusion, we present an outlook on future studies of attosecond dynamics in liquids.
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published
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Ultrafast Electronic and Structural Dynamics
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73 - 117
Publisher
Springer
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03888 - Wörner, Hans Jakob / Wörner, Hans Jakob
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Funding
307270 - Measuring attosecond electron dynamics in molecules (EC)
772797 - Attosecond X-ray spectroscopy of liquids (EC)
159875 - Attosecond transient-absorption spectroscopy of electronic dynamics in molecules (SNF)
172946 - Soft-X-ray spectroscopy on the attosecond time scale (SNF)
204928 - Attosecond chemistry in the gas and liquid phases (SNF)
772797 - Attosecond X-ray spectroscopy of liquids (EC)
159875 - Attosecond transient-absorption spectroscopy of electronic dynamics in molecules (SNF)
172946 - Soft-X-ray spectroscopy on the attosecond time scale (SNF)
204928 - Attosecond chemistry in the gas and liquid phases (SNF)