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Nonlinear Optics

A strong-field-ionization-enabled temporal gate for resolving ultrafast dynamics

Alexander Blättermann, Andreas Kaldun, Veit Stooß, Stefan Donsa, Hui Li Wei, Renate Pazourek, Stefan Nagele, C. Ott, C. D. Lin, Joachim Burgdörfer, Thomas Pfeifer

Published Jan 1, 2017• 0 citations
Publisher

Abstract

We create a tunable temporal gate by strong-field depletion of a previously excited two-electron system. This allows us to temporally resolve the emergence of a Fano resonance – a longstanding quest in attosecond science.
DOI
10.1364/nlo.2017.nth1a.3

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The goal of this work is to study and understand dynamics of atomic systems interacting with strong fields. To this end, a method referred to as strong-field spectroscopy is used, which measures the absorption spectrum of atoms interacting with such fields. In the scope of this work, a technique which allows the simultaneous measurement of absorption spectra of attosecond pulses and their reference signal is developed, which significantly increases the sensitivity to absorption changes. Additionally, a reconstruction method is introduced which retrieves the time-dependent evolution of the dipole response of an atomic system directly from a single absorption spectrum. Strong-field spectroscopy combines these techniques to examine the nonlinear strong-field dynamics in atomic and molecular systems and is applied to study the strongly correlated doubly excited states in helium. Furthermore, a measurement approach is introduced which uses the interaction with a high-intensity laser pulse to impose a time gate on the evolution of the coherent response of a system, which has previously been excited by an ultrashort laser pulse. With this approach the buildup of resonance phenomena in a wide range of physical systems can be studied. As a first application, the time-dependent buildup of a Fano resonance as well as the buildup of a whole Rydberg series are investigated.
We report on the experimental observation of the buildup of the 2s2p Fano resonance in helium in the time domain, which has been under theoretical investigation for more than a decade. The emergence of the absorption line is temporally resolved by interrupting the natural decay of the excited state via saturated strong-field ionization at a variable time delay. We compare the experimental data with full ab-initio simulations to validate the time-gating by strong-field ionization and thereby confirm the recently developed theory for the formation of Fano line-profiles.
Attosecond time-resolved electron tunneling dynamics have been investigated by using attosecond angular streaking spectroscopy, where a clock reference to the laser field vector is required in atomic strong-field ionization and the situation becomes complicated in molecules. Here we reveal a resonant ionization process via a transient state by developing an electron-tunneling-site-resolved molecular attoclock in Ar-Kr^{+}. Two distinct deflection angles are observed in the photoelectron angular distribution in the molecular frame, corresponding to the direct and resonant ionization pathways. We find the electron is temporally trapped in the Coulomb potential wells of the Ar-Kr^{+} before finally releasing into the continuum when the electron tunnels through the internal barrier. By utilizing the direct tunneling ionization as a self-referenced arm of the attoclock, the time delay of the electron trapped in the resonant state is revealed to be 3.50±0.04 fs. Our results give an impetus to exploring the ultrafast electron dynamics in complex systems and also endow a semiclassical presentation of the electron trapping dynamics in a quantum resonant state.