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We present theoretical studies on real-time probing of the electron density evolution of an atom in a strong infrared (IR) laser field with few-cycle near-infrared (NIR) and attosecond extreme-ultraviolet (XUV) pulses. Our results indicate that the electron density near the tunneling barrier is reflected in the additional tunneling ionization yield with a time delayed NIR pulse and the electron density near the nucleus can be probed by the single photoionization yield with a time delayed XUV pulse. It turns out the NIR-probing scheme can be used to study the polarization of the system in an external IR field and the XUV probing can be additionally applied to explore excitation dynamics during and after the IR field interaction. [ABSTRACT FROM AUTHOR]

We study laser-sub-cycle control over electron trajectories concomitantly in space and time using orthogonally polarized two-color laser fields. We compare experimental photoelectron spectra of neon recorded by coincidence momentum imaging with photoelectron spectra obtained by semiclassical and numerical solutions of the time-dependent Schrödinger equation. We find that a resolution of a quarter optical cycle in the photoelectron trajectories can be achieved. It is shown that depending on their sub-cycle birth time the trajectories of photoelectrons are affected differently by the ion's Coulomb field. [ABSTRACT FROM AUTHOR]

We experimentally investigate the ionization mechanism behind the formation of remarkably high charge states observed in the laser-pulse-induced fragmentation of different hydrocarbon molecules by Roither et al. [Phys. Rev. Lett. 106. 163001 (2011)], who suggested enhanced ionization occurring at multiple C-H bonds as the underlying ionization mechanism. Using multiparticle coincidence momentum imaging we measure the yield of multiply charged fragmenting ethylene and acetylene molecules at several intensities and pulse durations ranging from the few-cycle regime to 25 fs. We observe, at constant intensity, a strong increase of the proton energy with increasing laser pulse duration. It is shown that this is caused by a strong increase in the yield of highly charged parent molecular ions with pulse duration. Based on experimental evidence we explain this increase by the necessary population of precursor states in the parent ion that feature fast C-H stretch dynamics to the critical internuclear distance, where efficient ionization via enhanced ionization takes place. For increasing pulse duration these precursor ionic states are more efficiently populated, which leads in turn to a higher enhanced-ionization probability for longer pulses. Our work provides experimental evidence for the existence of a multiple-bond version of enhanced ionization in polyatomic molecules. [ABSTRACT FROM AUTHOR]

We present measured momentum distributions on the double ionization of helium with intense, near-circularly-polarized few-cycle laser pulses with a known carrier-envelope offset phase (CEP). The capability of obtaining CEP-resolved momentum distributions enables us to observe signatures of the various combinations of laser-half-cycle two-electron emissions. By comparison to semiclassical trajectory simulations, we succeed in assigning the corresponding structures in the measured distributions to certain two-electron emission dynamics. Based on this possibility, we demonstrate that the sequential double-ionization dynamics can be sensitively controlled with the pulse duration and the laser peak intensity. For the shortest pulse durations and not too high intensities we find that the two electrons are dominantly emitted with a delay of roughly a laser half cycle. For a just slightly increased intensity we find evidence that at least one of the two electrons is surprisingly likely emitted in between the peaks of the laser field oscillations rather than at the field maxima. The simulations reproduce the signatures of these kinds of two-electron emissions overall relatively well. [ABSTRACT FROM AUTHOR]

The alignment-dependent ionization of acetylene and ethylene in short laser pulses is investigated in the framework of the time-dependent density-functional theory coupled with Ehrenfest dynamics. The molecular alignment is found to have a substantial effect on the total ionization. Bond stretching is shown to cause an increase of the ionization efficiency, i.e., enhanced ionization, in qualitative agreement with previous theoretical investigations. It is also demonstrated that the enhanced ionization mechanism greatly enhances the ionization from the inner valence orbitals, and the ionization of the inner orbitals is primarily due to their extended weakly bound density tails. [ABSTRACT FROM AUTHOR]

We present a theoretical analysis of the atomic photoelectron emission spectra produced by a linearly polarized sculpted laser pulse of two colors with frequencies ω and 2ω. The spectrum of the "direct" electrons with intermediate energies prominently features both intracycle and intercycle interferences. We derive a simple analytic expression for this spectral range based on a semiclassical approximation of the time-dependent distorted wave strong-field approximation generalized to strong-field ionization by a two-color pulse. We verify its applicability to approximately represent the intricate interference patterns by comparison with the exact solutions of the time-dependent Schrödinger equation and with the strong-field approximation. We show that the interference patterns can be tuned and its contrast enhanced by the additional "knob" available, the relative phase between the two frequency components. The present results confirm that two-color ionization allows resolving interference structures originating from trajectories launched within a time interval of less than 100 as [X. Xie, Phys. Rev. Lett. 108, 193004 (2012)]. [ABSTRACT FROM AUTHOR]

Field ionization and Coulomb explosion of small hydrocarbon molecules driven by intense laser pulses are studied in a combined theoretical and experimental framework. The spectra of ejected protons calculated by the time-dependent density functional approach are in good agreement with the experimental data. The results of the simulations give detailed insight into the correlated electron and nuclear dynamics and complement the experiment with a time-dependent physical picture. It is demonstrated that the Coulomb explosion in the studied molecular systems is a sudden, all-at-once fragmentation where the ionization step is followed by a simultaneous ejection of the charged fragments. [ABSTRACT FROM AUTHOR]

We demonstrate control over the localization of high-lying Rydberg wave packets in argon atoms with phase-locked orthogonally polarized two-color laser fields. With a reaction microscope, we measure ionization signals of high-lying Rydberg states induced by a weak dc field and blackbody radiation as a function of the relative phase between the two-color fields. We find that the dc-field-ionization yield of high-lying Rydberg argon atoms oscillates with the relative two-color phase with a period of 2π while the photoionization signal by blackbody radiation shows a period of π. Accompanying simulations show that these observations are a clear signature of the asymmetric localization of electrons recaptured into very elongated (low angular momentum) high-lying Rydberg states after conclusion of the laser pulse. Our findings thus open an effective pathway to control the localization of high-lying Rydberg wave packets. [ABSTRACT FROM AUTHOR]

We investigate sequential double ionization of helium by intense near-circularly polarized few-cycle laser pulses using a semiclassical ionization model with two independent electrons. Simulated He2+ ion momentum distributions are compared to those obtained in recent benchmark experiments [M. S. Schöffler, X. Xie, P. Wustelt, M. Möller, S. Roither, D. Kartashov, A. M. Sayler, A. Baltuska, G. G. Paulus, and M. Kitzler, Phys. Rev. A 93, 063421 (2016)]. We study the influence of a number of pulse parameters such as peak intensity, carrier-envelope phase, pulse duration, and second- and third-order spectral phase on the shape of the ion momentum distributions. Good agreement is found in the main features of these distributions and of their dependence on the laser pulse duration, peak intensity, and carrier-envelope phase. Furthermore, we find that for explaining certain fine-scale features observed in the experiments, it becomes important to consider subtle timing variations in the two-electron emissions introduced by small values of chirp. This result highlights the possibility of measuring and controlling multielectron dynamics on the attosecond time scale by fine tuning the field evolution of intense close-to-single-cycle laser pulses. [ABSTRACT FROM AUTHOR]

We report experiments on the direct observation of molecular oxygen formation from CO2 in strong laser fields with a reaction microscope. Our accompanying simulations and pump-probe measurements suggest that CO2 molecules undergo bending motion during strong-field ionization which supports the molecular oxygen formation process. The observation of molecular oxygen formation from CO2 may trigger further experimental and theoretical studies on such processes with laser pulses, and provides hints in studies of the O2 and O2+ abundance in CO2-dominated planetary atmospheres. [ABSTRACT FROM AUTHOR]

We demonstrate the detection of high-lying Rydberg states produced in strong laser fields with coincidence spectroscopy. Electron emission after the interaction of strong laser pulses with atoms and molecules is measured together with the parent ions in coincidence measurements. These electrons originate from high-lying Rydberg states with quantum numbers from n~20 up to n≲120 formed by frustrated field ionization. Ionization rates are retrieved from the measured ionization signal of these Rydberg states. Simulations show that both tunneling ionization by a weak dc field and photoionization by blackbody radiation contribute to delayed electron emission on the nano- to microsecond scale. Furthermore, the dependence of the Rydberg-state production on the ellipticity of the driving laser field indicates that such high-lying Rydberg states are populated through electron recapture. The present experiment provides detailed quantitative information on Rydberg production in strong-field interaction. [ABSTRACT FROM AUTHOR]

We experimentally and theoretically investigated the deprotonation process on nanosecond to microsecond timescales in ethylene and acetylene molecules following their double ionization by a strong femtosecond laser field. In our experiments we utilized coincidence detection with the reaction microscope technique. We found that both the lifetime of the long-lived ethylene dication leading to the delayed deprotonation and the relative channel strength of the delayed deprotonation compared to the prompt one have no evident dependence on the laser pulse duration and the laser peak intensity. Quantum chemical simulations suggest that the observed delayed fragmentation process originates from the tunneling from near-dissociation-threshold C-H stretch vibrational states on a dicationic electronic state. These vibrational states can be populated through strong field double-ionization-induced vibrational excitation on an electronically excited state in the case of ethylene, and through a spin-flip transition from electronically excited singlet states to the triplet ground state in the case of acetylene. [ABSTRACT FROM AUTHOR]