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All-optical Stückelberg spectroscopy of strongly driven Rydberg states
2022, Bengs, Ulrich, Patchkovskii, Serguei, Ivanov, Misha, Zhavoronkov, Nickolai
The AC Stark shift of electronic levels is ubiquitous in the interaction of intense light fields with atoms and molecules. As the light intensity changes on the rising and falling edges of a femtosecond laser pulse, it shifts the Rydberg states in and out of multiphoton resonances with the ground state. The two resonant pathways for transient excitation arising at the leading and the trailing edges of the pulse generate Young's type interference, generally referred to as the Stückelberg oscillations. Here we report the observation of the Stückelberg oscillations in the intensity of the coherent free-induction decay following resonant multiphoton excitation. Moreover, combining the experimental results with accurate numerical simulations and a simple model, we use the Stückelberg oscillations to recover the population dynamics of strongly driven Rydberg states inside the laser pulse by all-optical measurements after the end of the pulse. We demonstrate the potential of this spectroscopy to characterize lifetimes of Rydberg states dressed by laser fields with strengths far exceeding the Coulomb field between the Rydberg electron and the core.
Electron dynamics in laser-driven atoms near the continuum threshold
2021, Liu, Mingqing, Xu, Songpo, Hu, Shilin, Becker, Wilhelm, Quan, Wei, Liu, Xiaojun, Chen, Jing
Strong-field ionization and Rydberg-state excitation (RSE) near the continuum threshold exhibit two phenomena that have attracted a lot of recent attention: the low-energy structure (LES) just above and frustrated tunneling ionization just below the threshold. The former becomes apparent for longer laser wavelengths, while the latter has been especially investigated in the near infrared; both have been treated as separate phenomena so far. Here we present a unified perspective based on electron trajectories, which emphasizes the very important role of the electron-ion Coulomb interaction as expected in this energy region. Namely, those trajectories that generate the LES can also be recaptured into a Rydberg state. The coherent superposition of the contributions of such trajectories with different travel times (each generating one of the various LES peaks) causes an oscillation in the intensity dependence of the RSE yield, which is especially noticeable for longer wavelengths. The theory is illustrated by RSE experiments at 1800 nm, which agree very well with the theory with respect to position and period of the oscillation. The wavelength scaling of the RSE oscillation is also discussed. Our work establishes a solid relationship between processes below and above the threshold and sheds new light on atomic dynamics driven by intense laser fields in this critical energy region.
Intracluster Coulombic decay following intense NIR ionization of clusters
2015, Schütte, Bernd, Arbeiter, Mathias, Fennel, Thomas, Jabbari, Ghazal, Gokhberg, Kirill, Kuleff, Alexander I., Vrakking, Marc J. J., Rouzée, Arnaud
We report on the observation of a novel intracluster Coulombic decay process following Rydberg atom formation in clusters ionized by intense near-infrared fields. A new decay channel emerges, in which a Rydberg atom relaxes to the ground state by transferring its excess energy to a weakly bound electron in the environment that is emitted from the cluster. We find evidence for this process in the electron spectra, where a peak close to the corresponding atomic ionization potential is observed. For Ar clusters, a decay time of 87 ps is measured, which is significantly longer than in previous time-resolved studies of interatomic Coulombic decay.
Correlated electronic decay following intense near-infrared ionization of clusters
2015, Schütte, Bernd, Arbeiter, Mathias, Fennel, Thomas, Jabbari, Ghazal, Kuleff, Alexander I., Vrakking, Marc J. J., Rouzée, Arnaud
We report on a novel correlated electronic decay process following extensive Rydberg atom formation in clusters ionized by intense near-infrared fields. A peak close to the atomic ionization potential is found in the electron kinetic energy spectrum. This new contribution is attributed to an energy transfer between two electrons, where one electron decays from a Rydberg state to the ground state and transfers its excess energy to a weakly bound cluster electron in the environment that can escape from the cluster. The process is a result of nanoplasma formation and is therefore expected to be important, whenever intense laser pulses interact with nanometer-sized particles.