Adrian N. Pfeiffer

Attosecond ionization and tunneling delay time measurements in helium.

It is well established that electrons can escape from atoms through tunneling under the influence of strong laser fields, but the timing of the process has been controversial and far too rapid to probe in detail. We used attosecond angular streaking to place an upper limit of 34 attoseconds and an intensity-averaged upper limit of 12 attoseconds on the tunneling delay time in strong field ionization of a helium atom. The ionization field derives from 5.5-femtosecond-long near-infrared laser pulses with peak intensities ranging from 2.3 × 1014 to 3.5 × 1014 watts per square centimeter (corresponding to a Keldysh parameter variation from 1.45 to 1.17, associated with the onset of efficient tunneling). The technique relies on establishing an absolute reference point in the laboratory frame by elliptical polarization of the laser pulse, from which field-induced momentum shifts of the emergent electron can be assigned to a temporal delay on the basis of the known oscillation of the field vector.

Probing the longitudinal momentum spread of the electron wave packet at the tunnel exit.

We present an ellipticity resolved study of momentum distribution arising from strong-field ionization of helium. The influence of the ion potential on the departing electron is considered within a semi-classical model consisting of an initial tunneling step and subsequent classical propagation. We find that the momentum distribution can be explained by including the longitudinal momentum spread of the electron at the exit from the tunnel. Our combined experimental and theoretical study provides an estimate of this momentum spread.

Rydberg state creation by tunnel ionization

It is well known from numerical and experimental results that the fraction of Rydberg states (excited neutral atoms) created by tunnel ionization declines dramatically with increasing ellipticity of laser light, in a way that is similar to high harmonic generation (HHG). We present a method to analyze this dependence on ellipticity, deriving a probability distribution of Rydberg states that agrees closely with experimental (Nubbemeyer et al 2008 Phys. Rev. Lett. 101 233001) and numerical results. We show using analysis and numerics that most Rydberg electrons are ionized before the peak of the electric field and therefore do not come back to the parent ion. Our work shows, for the first time, the similarities and differences in the process that distinguishes formation of Rydberg electrons from electrons involved in HHG: ionization occurs in a different part of the laser cycle, but the post-ionization dynamics are very similar in both cases, explaining why the same dependence on ellipticity is observed.

Recent attoclock measurements of strong field ionization

Abstract The attoclock is a powerful, new, and unconventional experimental tool to study fundamental attosecond dynamics on an atomic scale. We have demonstrated the first attoclock with the goal to measure the tunneling delay time in laser-induced ionization of helium and argon atoms, with surprising results. It was found that the time delay in tunneling is zero for helium and argon atoms within the experimental uncertainties of a few 10’s of attoseconds. Furthermore we showed that the single active electron approximation is not sufficient even for atoms such as argon and the parent-ion interaction is much more complex than normally assumed. For double ionization of argon we found again surprising results because the ionization time of the first electron is in good agreement with the predictions, whereas the ionization of the second electron occurs significantly earlier than predicted and the two electrons exhibit some unexpected correlation.We present an ellipticity-resolved study of momentum distributions arising from strong-field ionization of helium. The influence of the ion potential on the departing electron is considered within a semiclassical model consisting of an initial tunneling step and subsequent classical propagation. We find that the momentum distribution can be explained by including the longitudinal momentum spread of the electron at the exit from the tunnel. Our combined experimental and theoretical study provides an estimate of this momentum spread.

Comparison of different approaches to the longitudinal momentum spread after tunnel ionization

We introduce a method to investigate the longitudinal momentum spread resulting from strong-field tunnel ionization of helium which, unlike other methods, is valid for all ellipticities of laser pulse. Semiclassical models consisting of tunnel ionization followed by classical propagation in the combined ion and laser field reproduce the experimental results if an initial longitudinal spread at the tunnel exit is included. The values for this spread are found to be of the order of twice the transverse momentum spread.

Strong-field induced XUV transmission and multiplet splitting in 4d−16p core-excited Xe studied by femtosecond XUV transient absorption spectroscopy

Light-induced coupling of core-excited states of Xe atoms is investigated by femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy with photon energies ranging from 50 eV to 72 eV. Coupling of the 4d(-1)((2)D(5/2))6p((2)P(3/2)) (65.1 eV) and 4d(-1)((2)D(3/2))6p((2)P(1/2)) (67.0 eV) core-excited states to nearby states by a strong infrared laser field leads to a threefold enhancement of XUV transmission. The transmission at 65.1 eV (67.0 eV) changes from 3.2 ± 0.4% (5.9 ± 0.5%) without the coupling laser to 9 ± 2% (22 ± 5%) at the maximum of the laser field. A strong-field induced broad XUV absorption feature between 60 eV and 65 eV is ascribed to splitting of the field-free absorption lines into multiple branches when the Rabi frequencies of the coupling transitions exceed the infrared laser frequency. This picture is supported by a comparison of the strong-field induced absorption spectrum with a numerical integration of the von Neumann equation for a few-level quantum system. The valence hole-alignment of strong-field ionized Xe is revisited, confirming the previously observed reduced alignment compared to theoretical predictions.

Subcycle-resolved probe retardation in strong-field pumped dielectrics

The response of a bulk dielectric to an intense few-cycle laser pulse is not solely determined by the pulse envelope, but also by ultrafast processes occuring during each optical cycle. Here, a method is presented for measuring the retardation of a probe pulse in a strong-field pumped, bulk dielectric with subcycle resolution in the pump–probe delay. Comparisons to model calculations show that the measurement is sensitive to the timing of the electronic Kerr response. When conduction band states are transiently populated at the crests of the laser field, the measurement is also sensitive to the interband dephasing time.

Investigation of coupling mechanisms in attosecond transient absorption of autoionizing states: comparison of theory and experiment in xenon

© 2015 IOP Publishing Ltd. Attosecond transient absorption spectra near the energies of autoionizing states are analyzed in terms of the photon coupling mechanisms to other states. In a recent experiment, the autoionization lifetimes of highly excited states of xenon were determined and compared to a simple expression based on a model of how quantum coherence determines the decay of a metastable state in the transient absorption spectrum. Here it is shown that this procedure for extracting lifetimes is more general and can be used in cases involving either resonant or nonresonant coupling of the attosecond-probed autoionizing state to either continua or discrete states by a time-delayed near infrared (NIR) pulse. The fits of theoretically simulated absorption signals for the 6p resonance in xenon (lifetime = 21.1 fs) to this expression yield the correct decay constant for all the coupling mechanisms considered, properly recovering the time signature of twice the autoionization lifetime due to the coherent nature of the transient absorption experiment. To distinguish between these two coupling cases, the characteristic dependencies of the transient absorption signals on both the photon energy and time delay are investigated. Additional oscillations versus delay-time in the measured spectrum are shown and quantum beat analysis is used to pinpoint the major photon-coupling mechanism induced by the NIR pulse in the current xenon experiment: the NIR pulse resonantly couples the attosecond-probed state, 6p, to an intermediate 8s (at 22.563 eV), and this 8s state is also coupled to a neighboring state (at 20.808 eV).

Calculation of valence electron motion induced by sequential strong-field ionisation

Strong-field ionisation leads to the formation of electron wave packets in the valence shell of the resulting ion under appropriate experimental conditions. Ab-initio calculations of the population and coherence dynamics are challenging and are usually limited to single ionisation of simple systems by linearly polarised fields. Here, a calculation based on static-field rate equations is presented to obtain the density matrix for sequential double ionisation. The results for single ionisation of neon and xenon by linearly polarised pulses are in satisfactory agreement with ab-initio calculations. For double ionisation of neon and xenon by elliptically polarised fields, five coherence channels with recurrence times between 1.1 fs and 51.9 fs are predicted to exhibit a significant degree of coherence. The degree of coherence is affected by the polarisation of the laser pulse and decreases in general for elliptical polarisation, but for the investigated cases a significant degree of coherence is predicted to occur up to the regime of close-to-circular polarisation.

The Attoclock: A Novel Ultrafast Measurement Technique with Attosecond Time Resolution

The recent progress of the ultrafast laser technology enables to capture and control electrons dynamics, which is the key to understand how energy and charge are transported not only in atoms but also in more complex solid-state and molecular systems. This task calls for the development of novel measurement techniques with attosecond time resolution. The “attoclock” is a relatively simple method, which provides attosecond time resolution without the explicit need of attosecond pulses. In this chapter we review the details of this powerful experimental technique, which was employed in the recent years to investigate electron tunneling dynamics and to study the electron kinematics in strong field single and double ionization.