Characterization of vacuum and deep ultraviolet pulses via two-photon autocorrelation signals.

Characterization of ultrashort vacuum and deep ultraviolet pulses is important in view of applications of those pulses for spectroscopic and dynamical imaging of atoms, molecules, and materials. We present an extension of the autocorrelation technique, applied for measurement of the pulse duration via a single Gaussian function. Analytic solutions for two-photon ionization of atoms by Gaussian pulses are used along with an expansion of the pulse to be characterized using multiple Gaussians at multi-color central frequencies. This approach allows one to use two-photon autocorrelation signals to characterize isolated ultrashort pulses and pulse trains, i.e., the time-dependent amplitude and phase variation of the electric field. The potential of the method is demonstrated using vacuum and deep ultraviolet pulses and pulse trains obtained from numerical simulations of macroscopic high harmonic spectra.

Asymmetries in ionization of atomic superposition states by ultrashort laser pulses.

Progress in ultrafast science allows for probing quantum superposition states with ultrashort laser pulses in the new regime where several linear and nonlinear ionization pathways compete. Interferences of pathways can be observed in the photoelectron angular distribution and in the past they have been analyzed for atoms and molecules in a single quantum state via anisotropy and asymmetry parameters. Those conventional parameters, however, do not provide comprehensive tools for probing superposition states in the emerging research area of bright and ultrashort light sources, such as free-electron lasers and high-order harmonic generation. We propose a new set of generalized asymmetry parameters which are sensitive to interference effects in the photoionization and the interplay of competing pathways as the laser pulse duration is shortened and the laser intensity is increased. The relevance of the parameters is demonstrated using results of state-of-the-art numerical solutions of the time-dependent Schrödinger equation for ionization of helium atom and neon atom.

Macroscopic properties of high-order harmonic generation from molecular ions.

High harmonic spectroscopy utilizes the extremely nonlinear optical process of high-order harmonic generation (HHG) to measure complex attosecond-scale dynamics within the emitting atom or molecule subject to a strong laser field. However, it can be difficult to compare theory and experiment, since the dynamics under investigation are often very sensitive to the laser intensity, which inevitably varies over the Gaussian profile of a typical laser beam. This discrepancy would usually be resolved by so-called macroscopic HHG simulations, but such methods almost always use a simplified model of the internal dynamics of the molecule, which is not necessarily applicable for high harmonic spectroscopy. In this Letter, we extend the existing framework of macroscopic HHG so that high-accuracy ab initio calculations can be used as the microscopic input. This new (to the best of our knowledge) approach is applied to a recent theoretical prediction involving the HHG spectra of open-shell molecules undergoing nonadiabatic dynamics. We demonstrate that the predicted features in the HHG spectrum unambiguously survive macroscopic response calculations, and furthermore they exhibit a nontrivial angular pattern in the far field.

Isolated broadband attosecond pulse generation with near- and mid-infrared driver pulses via time-gated phase matching.

We present a theoretical analysis of the time-gated phase matching (ionization gating) mechanism in high-order harmonic generation for the isolation of attosecond pulses at near-infrared and mid-infrared driver wavelengths, for both few-cycle and multi-cycle driving laser pulses. Results of our high harmonic generation and three-dimensional propagation simulations show that broadband isolated pulses spanning from the extreme-ultraviolet well into the soft X-ray region of the spectrum can be generated for both few-cycle and multi-cycle laser pulses. We demonstrate the key role of absorption and group velocity matching for generating bright, isolated, attosecond pulses using long wavelength multi-cycle pulses. Finally, we show that this technique is robust against carrier-envelope phase and peak intensity variations.

Zeptosecond high harmonic keV x-ray waveforms driven by midinfrared laser pulses.

We demonstrate theoretically that the temporal structure of high harmonic x-ray pulses generated with midinfrared lasers differs substantially from those generated with near-infrared pulses, especially at high photon energies. In particular, we show that, although the total width of the x-ray bursts spans femtosecond time scales, the pulse exhibits a zeptosecond structure due to the interference of high harmonic emission from multiple reencounters of the electron wave packet with the ion. Properly filtered and without any compensation of the chirp, regular subattosecond keV waveforms can be produced.

Enhancement of vibrational excitation and dissociation of H2(+) in infrared laser pulses.

We study vibrational excitations, dissociation, and ionization of H(2)(+) in few-cycle laser pulses over a broad wavelength regime. Our results of numerical simulations supported by model calculations show a many orders-of-magnitude enhancement of vibrational excitation and dissociation (over ionization) of the molecular ion at infrared wavelengths. The enhancement occurs without any chirping of the pulse, which was previously applied to take account of the anharmonicity of the molecular vibrations. The effect is related to strong-field two- and higher-order photon transitions between different vibrational states.

Nonequilibrium evolution of strong-field anisotropic ionized electrons towards a delayed plasma-state.

Rigorous quantum calculations of the femtosecond ionization of hydrogen atoms in air lead to highly anisotropic electron and ion angular (momentum) distributions. A quantum Monte-Carlo analysis of the subsequent many-body dynamics reveals two distinct relaxation steps, first to a nearly isotropic hot nonequilibrium and then to a quasi-equilibrium configuration. The collective isotropic plasma state is reached on a picosecond timescale well after the ultrashort ionizing pulse has passed.

Wavelength dependence of the suppressed ionization of molecules in strong laser fields.

We study ionization of molecules by an intense laser field over a broad wavelength regime, ranging from 0.8 to 1.5 µm experimentally and from 0.6 to 10 µm theoretically. A reaction microscope is combined with an optical parametric amplifier to achieve ionization yields in the near-infrared wavelength regime. Calculations are done using the strong-field S-matrix theory and agreement is found between experiment and theory, showing that ionization of many molecules is suppressed compared to the ionization of atoms with identical ionization potentials at near-infrared wavelengths at around 0.8 µm, but not at longest wavelengths (10 µm). This is due to interference effects in the electron emission that are effective at low photoelectron energies but tend to average out at higher energies. We observe the transition between suppression and nonsuppression of molecular ionization in the near-infrared wavelength regime (1-5 µm).

Single-active-electron ionization of C60 in intense laser pulses to high charge states.

Sequential ionization of the C(60) fullerene to high charge states in ultrashort intense laser pulses is investigated within the strong-field S-matrix approach. Ion yields are calculated and saturation intensities are determined for a broad range of laser wavelengths between 395 and 1800 nm at different pulse lengths. Comparisons of the S-matrix predictions for the saturation intensities with recent experimental data are in an overall satisfactory agreement, indicating that saturation of ionization of this complex molecule can be well described using the single-active-electron approach. The analysis of the results shows that the contributions from the h(u)-highest occupied molecular orbital to the ion yields dominate as compared to those from the inner valence shells h(g) and g(g). Finally, it is demonstrated that the suppression of ionization of C(60) and its ions, as observed in experiments, can be interpreted within the present theory as due to the finite cage size of the fullerenes and a multi-slit-like interference effect between partial waves emitted from the different nuclei of the fullerenes.

Saturated ionization of fullerenes in intense laser fields.

We investigate the ionization of icosahedral fullerenes (C20, C60, C80, and C180) in an intense laser pulse using the S-matrix theory. The results obtained are in excellent agreement with the recent observations of unexpectedly high saturation intensities of the Buckminster fullerene and its multiply charged ions. Our analysis strongly suggests that the related phenomenon of suppressed ionization of these complex fullerenes is due to the finite cage size and the "multislit" interference effect between partial waves emitted from the different nuclei rather than to a dynamical multielectron polarization effect.