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We demonstrate a time-domain method to quantitatively retrieve the angular dependence of laser-induced electron rescattering from the measured rotational half-revival signals of molecules with a reaction microscope. The method is based on the measured channel-resolved ion yields of single ionization and electron-rescattering-induced double ionization and the in situ measured alignment distribution of molecules. From the measured data for ${\mathrm{CO}}_{2}$, we retrieve the angular dependence of electron rescattering in nonsequential double ionization for both nondissociative and dissociative cases. The results imply that the angular dependence of electron rescattering is affected by the state of the parent ion populated during the first ionization step. The method demonstrated here opens up the possibility to quantitatively retrieve from measured data which molecular orbitals are involved in the interaction of strong laser fields with molecules.

Laser induced x-ray fluorescence were observed against laser polarization ellipticity. While emission from krypton peaks at linear polarization, a signature of recollision, emission from neon shows opposite trend. We attribute it to two competing processes.

The authors use time-domain spectroscopy with attosecond X-ray pulses to access the time and energy information of rescattering electrons simultaneously.

We describe the results of experiments and simulations performed with the aim of extending photoelectron spectroscopy with intense laser pulses to the case of molecular compounds. Dimer frame photoelectron angular distributions generated by double ionization of ${\mathrm{N}}_{2}\ensuremath{-}{\mathrm{N}}_{2}$ and ${\mathrm{N}}_{2}\ensuremath{-}{\mathrm{O}}_{2}$ van der Waals dimers with ultrashort, intense laser pulses are measured using four-body coincidence imaging with a reaction microscope. To study the influence of the first-generated molecular ion on the ionization behavior of the remaining neutral molecule we employ a two-pulse sequence comprising of a linearly polarized and a delayed elliptically polarized laser pulse that allows distinguishing the two ionization steps. By analysis of the obtained electron momentum distributions we show that scattering of the photoelectron on the neighboring molecular potential leads to a deformation and rotation of the photoelectron angular distribution as compared to that measured for an isolated molecule. Based on this result we demonstrate that the electron momentum space in the dimer case can be separated, allowing us to extract information about the ionization pathway from the photoelectron angular distributions. Our work, when implemented with a variable pulse delay, opens up the possibility of investigating light-induced electronic dynamics in molecular dimers using angularly resolved photoelectron spectroscopy with intense laser pulses.

We establish a generalized picture of the phase sensitivity of laser-induced directional bond breaking using the H_{2} molecule as the example. We show that the well-known proton ejection anisotropy measured with few-cycle pulses as a function of their carrier-envelope phases arises as an amplitude modulation of an intrinsic anisotropy that is sensitive to the laser phase at the ionization time and determined by the molecule's electronic structure. Our work furthermore reveals a strong electron-proton correlation that may open up a new approach to experimentally accessing the laser-sub-cycle intramolecular electron dynamics also in larger molecules.

We report on the unambiguous observation of the subcycle ionization bursts in sequential strong-field double ionization of H_{2} and their disentanglement in molecular frame photoelectron angular distributions. This observation was made possible by the use of few-cycle laser pulses with a known carrier-envelope phase, in combination with multiparticle coincidence momentum imaging. The approach demonstrated here will allow sampling of the intramolecular electron dynamics and the investigation of charge-state-specific Coulomb distortions on emitted electrons in polyatomic molecules.

This works shows a new approach to study the electron recapture process during double and multiple ionization of atoms. This scheme is applicable to non-dissociative processes in molecules, which are not accessible with existing methods based on the measurement of kinetic energy released from fragmentation processes. The experiments show a transition of frustrated double ionization in argon from a non-sequential scenario to a sequential scenario.

We report on the retrieval of the angular dependence of laser-induced electron rescattering in CO2 with a novel method from the measured rotational half revival signals of filed-free aligned molecules using a reaction microscope.

We report on the results of a joint experimental and numerical study on the sub-cycle laser field-driven electron dynamics that underlie the population of highly excited electronic states in multiply ionized argon dimers by electron recapture processes. Our experiments using few-cycle laser pulses with a known carrier-envelope phase (CEP) in combination with reaction microscopy reveal a distinct CEP-dependence of the electron emission and recapture process and, furthermore, a small but significant CEP-offset to the scenario in which no excited argon dimers are produced. With the help of classical ensemble trajectory simulations we trace down these different CEP-dependencies to subtle differences in the laser-driven sub-cycle electron trajectory dynamics that involve in both cases the transfer of an electron from one argon ion across the system boundary to the neighboring ion and its transient capture on this ion.

We experimentally investigate laser-induced dissociative recombination of CO$_2$ in linearly polarized strong laser fields with coincidence measurements. Our results show laser-induced dissociation processes originate from an electron recombination process after laser-induced double ionization. After double ionization of CO$_2$, one electron is recaptured by the CO$_2^{2+}$ and localized to O$^+$ or CO$^+$ in the following dissociation process. We found that the probability of electron localization to O$^{+}$ is much higher than that to CO$^+$. Further, our measurements reveal that the recombination probability of the first ionized electron is three times as high as that of the second ionized electron. Our work may trigger further experimental and theoretical studies on involved nuclear and electron dynamics in laser-induced dissociative recombination of molecules and their applications in controlling molecular dissociation with ultrashort laser pulses.

We experimentally investigate dissociation of ${\mathrm{H}}_{2}^{+}$ in the (near-)zero proton energy region. Based on our experimental results we conclude that the underlying mechanism for the production of protons with such low energy in strong two-color and broadband laser fields is a stimulated Raman-scattering-based zero-photon-dissociation process, ${\mathrm{ZPD}}_{\text{stR}}$, taking place on the electronic ground state. It is furthermore shown that in the (near-)zero energy region the asymmetry in proton ejection induced by asymmetric laser fields is due to the interplay of several processes, rather than only pathway interferences, with vibrational trapping (or bond hardening) taking a key role.

We demonstrate two-dimensional control over the chargelocalization in H2 dissociation using elliptically polarized laser pulses. The influences of the CEP and the laser phase at the instant of ionization are investigated.

The dynamics and the decay processes of inner-shell excited atoms are of great interest in physics, chemistry, biology, and technology. The highly excited state decays very quickly through different channels, both radiative and non-radiative. It is therefore a long-standing goal to study such dynamics directly in the time domain. Using few-cycle infrared laser pulses, we investigated the excitation and ionization of inner-shell electrons through laser-induced electron re-collision with the original parent ions and measured the dependence of the emitted x-ray spectra on the intensity and ellipticity of the driving laser. These directly re-colliding electrons can be used as the initiating pump step in pump/probe experiments for studying core-hole dynamics at their natural temporal scale. In our experiment we found that the dependence of the x-ray emission spectrum on the laser intensity and polarization state varies distinctly for the two kinds of atomic systems. Relying on our data and numerical simulations, we explain this behavior by the presence of different excitation mechanisms that are contributing in different ratios to the respective overall x-ray emission yields. Direct re-collision excitation competes with indirect collisions with neighboring atoms by electrons having "drifted away" from the original parent ion. (C) 2020 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

Many of the scientific applications for X-ray free-electron lasers seek to exploit the ultrashort pulse durations of intense X-rays to obtain femtosecond time resolution of various processes in a “pump-probe” scheme. One of the limiting factors for such experiments is the timing jitter between the X-rays and ultrashort pulses from more conventional lasers operating at near-optical wavelengths. In this work, we investigate the potential of using X-ray-induced changes in the optical second harmonic generation efficiency of a nonlinear crystal to retrieve single-shot arrival times of X-ray pulses with respect to optical laser pulses. Our experimental results and simulations show changes to the efficiency of the second harmonic generation of 12%, approximately three times larger than the measured changes in the transmission of the 800 nm center-wavelength fundamental pulse. Further experiments showing even larger changes in the transmission of 400 nm center-wavelength pulses show that the mechanism of the second harmonic generation efficiency modulation is mainly the result of X-ray-induced changes in the linear absorption coefficients near 400 nm. We demonstrate and characterize a cross-correlation tool based on this effect in reference to a previously demonstrated method of X-ray/optical cross-correlation.

We experimentally achieve two-dimensional CEP-control of bond breaking in H2 dissociation with elliptically polarized pulses. The lab and molecular frame of reference proton ejection asymmetries are compared.

We demonstrate kinematically complete measurements on frustrated double ionization of argon atoms in strong laser fields with a reaction microscope. We found that the electron trapping probability after strong field double ionization is much higher than that after strong field single ionization, especially in case of high laser intensity. The retrieved electron momentum distributions of frustrated double ionization show a clear transition from the nonsequential to the sequential regime, similar to those of strong field double ionization. The dependence of electron momentum width on the laser intensity further indicates that the second released electron has a dominant contribution to frustrated double ionization in the sequential regime.

We use orthogonally polarized two-color (OTC) laser pulses to separate quantum paths in the multiphoton ionization of Ar atoms. Our OTC pulses consist of 400 and 800 nm light at a relative intensity ratio of 10∶1. We find a hitherto unobserved interference in the photoelectron momentum distribution, which exhibits a strong dependence on the relative phase of the OTC pulse. Analysis of model calculations reveals that the interference is caused by quantum pathways from nonadjacent quarter cycles.

On the Earth, oxygen molecules are generated mostly via the photosynthesis by green plants and algae from carbon dioxide and water: nCO 2 + nH 2 O light→ (CH 2 O)n + nO 2 [1]. Although, theoretical studies showed the possibility of O 2 production via CO 2 fragmentation [2] and experimental investigations achieved the detection of C+ (referring the creation of O 2 on the other side) [3], the direct observation of O2 formation did not yet happen to our knowledge. In this submission, we report the direct experimental observation of molecular oxygen formation from carbon dioxide molecule after being doubly ionized by a strong laser pulse.

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 ${\mathrm{He}}^{2+}$ ion momentum distributions are compared to those obtained in recent benchmark experiments [M. S. Sch\"offler, X. Xie, P. Wustelt, M. M\"oller, 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.

Electron correlation in sequential double ionization of helium is studied experimentally with the ``attoclock'' technique. Control of the two-electron emission dynamics is demonstrated on the time scale of a half laser cycle.

We experimentally investigated a delayed fragmentation of hydrocarbon molecules on nanosecond to microsecond timescale after double ionization by femtosecond laser pulses. Quantum chemical simulations suggest that it originates from meta-stable high-lying vibrational states of dications.

Single and double electron recapture processes into Rydberg states driven by few-cycle laser pulses are studied for argon dimers. The electron emission and recapture dynamics show a strong dependence on the pulses’ carrier-envelope phase.

We report on the observation of subcycle interferences of electron wave packets released during strong field ionization of $\text{H}_{2}$ with cycle-shaped two-color laser fields. With a reaction microscope we measure three-dimensional momentum distributions of photoelectrons correlated with either $\text{H}_{2}^{+}$ or protons within different energy ranges generated by dissociation of $\text{H}_{2}^{+}$ . We refer to these different types of photoelectrons as channels. Our results show that the subcycle interference structures of electron wave packets are very sensitive to the cycle shape of the two-color laser field. We explain this behavior by the dependence of the ionization time within an optical cycle on the shape of the laser field cycle. The subcycle interference structures can be further used to obtain insight into the subcycle dynamics of molecules during strong field interaction.

The dynamics of sequential two-electron emission from helium is extracted from measured momentum distributions. Emission in between the field-maxima and on sub-laser-cycle times is identified. The corresponding structures are roughly reproduced by a semi-classical model.

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 $2\ensuremath{\pi}$ while the photoionization signal by blackbody radiation shows a period of $\ensuremath{\pi}$. 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.

Two-body dissociation processes of H2C@CH–CH@CH 2þ 2 induced by an intense laser field were investi

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.

We experimentally and theoretically show that by controlling the dynamics of removing three electrons from ethylene with ultrashort intense laser pulses allows for the determination of the relative probabilities for fragmentation into two respectively three molecular moieties.

We experimentally and theoretically demonstrate channel-selective control over strong-field induced fragmentation of a polyatomic molecule, acetylene, using impulsive laser alignment as the control mechanism.

Using orthogonally polarized two-color laser fields on neon and coincidence momentum imaging we gain access to the Coulomb influence in single ionization on sub-cycle times, and demonstrate a strong electron-electron anti-correlation in double ionization.

We demonstrate, using ethylene, that controlling lower-valence ionization and field-driven excitation dynamics with ultrashort, intense laser pulses allows steering fragmentation reactions of polyatomic molecules along a certain pathway towards a specific set of fragment ions.

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.

Double ionization of neon with orthogonally polarized two-color (OTC) laser fields is investigated using coincidence momentum imaging. We show that the two-electron emission dynamics in nonsequential double ionization can be controlled by tuning the subcycle shape of the electric field of the OTC pulses. We demonstrate experimentally switching from correlated to anticorrelated two-electron emission, and control over the directionality of the two-electron emission. Simulations based on a semiclassical trajectory model qualitatively explain the experimental results by a subcycle dependence of the electron recollision time on the OTC field shape. © 2014 American Physical Society.

The two-dimensional sub-cycle-time to electron momentum mapping provided by orthogonal two-color laser fields is applied to photoelectron spectroscopy. Using neon as the example we gain experimental access to the dynamics of emitted electron wave packets in electron momenta spectra measured by coincidence momentum imaging. We demonstrate the opportunities provided by this time-to-momentum mapping by investigating the influence of the parent ion on the emitted electrons on laser-sub-cycle times. It is found that depending on their sub-cycle birth time the trajectories of photoelectrons are affected differently by the ion's Coulomb field.

We experimentally demonstrated control of chemical bond break of ethylene in intense laser fields with employing both electronic dynamics and nuclear vibrational dynamics.

Control over various fragmentation reactions of a series of polyatomic molecules (acetylene, ethylene, 1,3-butadiene) by the optical waveform of intense few-cycle laser pulses is demonstrated experimentally. We show both experimentally and theoretically that the responsible mechanism is inelastic ionization from inner-valence molecular orbitals by recolliding electron wavepackets, whose recollision energy in few-cycle ionizing laser pulses strongly depends on the optical waveform. Our work demonstrates an efficient and selective way of pre-determining fragmentation and isomerization reactions in polyatomic molecules on sub-femtosecond time-scales.

We experimentally and theoretically demonstrate a self-referenced wave-function retrieval of a valence-electron wave packet during its creation by strong-field ionization with a sculpted laser field. Key is the control over interferences arising at different time scales. Our work shows that the measurement of subcycle electron wave-packet interference patterns can serve as a tool to retrieve the structure and dynamics of the valence-electron cloud in atoms on a sub-10-as time scale. Fil: Xie, Xinhua. Vienna University of Technology; Austria Fil: Roither, Stefan. Vienna University of Technology; Austria Fil: Kartashov, Daniil. Vienna University of Technology; Austria Fil: Persson, Emil. Vienna University of Technology; Austria Fil: Arbo, Diego. Consejo Nacional de Investigaciónes Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Astronomía y Física del Espacio. - Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Astronomía y Física del Espacio; Argentina. Vienna University of Technology; Austria Fil: Zhang, Li. Vienna University of Technology; Austria Fil: Gräfe, Stefanie. Vienna University of Technology; Austria Fil: Schöffler, Markus S.. Vienna University of Technology; Austria Fil: Burgdörfer, Joachim. Vienna University of Technology; Austria Fil: Baltuska, Andrius. Vienna University of Technology; Austria Fil: Kitzler, Markus. Vienna University of Technology; Austria

Atomic single- and double- ionization using orthogonally polarized two-color laser fields was investigated via COLTRILMS technique. We prove that the electronic wave packets can be spatially controlled with attosecond precision., 27th International Conference on Photonic, Electronic and Atomic Collisions, ICPEAC 2011, July 27 - August 2, 2011, Belfast, UK

Multiparticle coincidence imaging reveals laser-driven ejection of energetic protons via concerted Coulomb explosions from unexpectedly high molecular charge states. The underlying mechanism is studied with laser pulses from 4.5 to 27 fs in duration.

We manipulate the trajectories of field-ionizing electron wave packets using two-color laser pulses for controlling the Coulomb potential's influence on their three-dimensional momentum distributions.

Using multi-particle coincidence detection we are able to show that carbon-hydrogen molecules exposed to moderate laser-intensities can completely disintegrate from high charge states by a concerted emission of all protons with high kinetic energies.

Ultrafast proton migration in 1,3-butadiene in an intense laser field (40 fs, 4.5 × 10(14) W cm(-2)) is investigated by using Coulomb explosion coincidence momentum imaging. The spatial distribution maps of a migrating proton reconstructed for the two three-body Coulomb explosion pathways, C(4)H(6)(3+)→ H(+) + CH(3)(+) + C(3)H(2)(+) and C(4)H(6)(3+)→ H(+) + C(2)H(+) + C(2)H(4)(+), reveal that two protons migrate within a 1,3-butadiene molecule, prior to the three body decomposition.

We propose a general concept to use the spatial information encoded in the time-dependent polarization of high-order harmonic radiation generated by orthogonally polarized two-color laser fields. Based on polarization selective detection, we present two examples of applications: (i) a method for isolating a single attosecond pulse from an attosecond pulse train which is more efficient than the cutoff selection method and (ii) a technique for orbital tomography of molecules with attosecond resolution.

We report experimental observation of "slow" fragmentation from ethylene molecules on nanosecond or even microsecond timescale after their interaction with femtosecond laser pulses. Our results indicate that such fragmentation process originates from meta-stable high-lying vibrational states of ethylene ions.

By employing pump-probe back longitudinal diffractometry, the electron density and decay dynamics of a weak plasma channel created by a 1-KHz fs laser in air has been investigated. With ultrashort laser pulses of 50 fs and low energy of 0.6 mJ, we observe weak plasma channels with a length approximately 2 cm in air. An analytical reconstruction method of electron density has been analyzed, which is sensitive to the phase shift and channel size. The electron density in the weak plasma channel is extracted to be about 4 x 10(16) cm(-3). The diameters of the plasma channel and the filament are about 50 and 150 microm, respectively, and the measurable electron density can be extended to less than 10(15) cm(-3). Moreover, a different time-frequency technique called linearly chirped longitudinal diffractometry is proposed to time-resolved investigate ultrafast ionization dynamics of laser-irradiated gas, laser interaction with cluster beam, etc.

The scheme of high-intensity attosecond high-order harmonic generation driven by a synthesized laser field is proposed. The synthesized laser field is obtained by an appropriate superposition of a few-cycle laser pulse and a relatively long pulse of several tens of femtoseconds. Calculated results show that the intensity of the attosecond high-order harmonic pulse in helium driven by the synthesized laser field with a $8.8\ifmmode\times\else\texttimes\fi{}{10}^{13}\phantom{\rule{0.3em}{0ex}}\mathrm{W}∕{\mathrm{cm}}^{2}∕5\phantom{\rule{0.3em}{0ex}}\mathrm{fs}$ laser pulse and a $3.51\ifmmode\times\else\texttimes\fi{}{10}^{14}\phantom{\rule{0.3em}{0ex}}\mathrm{W}∕{\mathrm{cm}}^{2}∕50\phantom{\rule{0.3em}{0ex}}\mathrm{fs}$ laser pulse is several orders of magnitude higher than that driven by a single $8.8\ifmmode\times\else\texttimes\fi{}{10}^{13}\phantom{\rule{0.3em}{0ex}}\mathrm{W}∕{\mathrm{cm}}^{2}∕5\phantom{\rule{0.3em}{0ex}}\mathrm{fs}$ laser pulse, and it is even stronger than that driven by a single $7.9\ifmmode\times\else\texttimes\fi{}{10}^{14}\phantom{\rule{0.3em}{0ex}}\mathrm{W}∕{\mathrm{cm}}^{2}∕5\phantom{\rule{0.3em}{0ex}}\mathrm{fs}$ laser pulse, although the single and the synthesized pulses have the same peak electric-field strength.

We have studied the double ionization of Helium induced by intense (up to 1×1016 W/cm2) ultra-short (4-4.5 fs) circularly polarized laser pulses with a stabilized CEO phase.