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Stefan Pabst

Publications and source records attributed to Stefan Pabst.

25 records · Page 2Linked to original sources

Adiabaticity and diabaticity in strong-field ionization

If the photon energy is much less than the electron binding energy, ionization of an atom by a strong optical field is often described in terms of electron tunneling through the potential barrier resulting from the superposition of the atomic potential and the potential associated with the instantaneous electric component of the optical field. In the strict tunneling regime, the electron response to the optical field is said to be adiabatic, and nonadiabatic effects are assumed to be negligible. Here, we investigate to what degree this terminology is consistent with a language based on the so-called adiabatic representation. This representation is commonly used in various fields of physics. For electronically bound states, the adiabatic representation yields discrete potential energy curves that are connected by nonadiabatic transitions. When applying the adiabatic representation to optical strong-field ionization, a conceptual challenge is that the eigenstates of the instantaneous Hamiltonian form a continuum; i.e., there are no discrete adiabatic states. This difficulty can be overcome by applying an analytic-continuation technique. In this way, we obtain a rigorous classification of adiabatic states and a clear characterization of (non)adiabatic and (non)diabatic ionization dynamics. Moreover, we distinguish two different regimes within tunneling ionization and explain the dependence of the ionization probability on the pulse envelope.

physics.atom-ph↗

Theory of Attosecond Transient Absorption Spectroscopy of Krypton for Overlapping Pump and Probe Pulses

We present the first fully ab initio calculations for attosecond transient absorption spectroscopy of atomic krypton with overlapping pump and probe pulses. Within the time-dependent configuration interaction singles (TDCIS) approach, we describe the pump step (strong-field ionization using a near-infrared pulse) as well as the probe step (resonant electron excitation using an extreme- ultraviolet pulse) from first principles. We extent our TDCIS model and account for the spin-orbit splitting of the occupied orbitals. We discuss the spectral features seen in a recent attosecond transient absorption experiment [A. Wirth et al., Science 334, 195 (2011)]. Our results support the concept that the transient absorption signal can be directly related to the instantaneous hole population even during the ionizing pump pulse. Furthermore, we find strong deformations in the absorption lines when the overlap of pump and probe pulses is maximum. These deformations can be described by relative phase shifts in the oscillating ionic dipole. We discuss possible mechanisms contributing to these phase shifts. Our finding suggests that the non-perturbative laser dressing of the entire N -electron wave function is the main contributor.

physics.atom-ph↗

Enhanced nonlinear response of Ne$^{8+}$ to intense ultrafast x rays

We investigate the possible reasons for the discrepancy between the theoretical two-photon ionization cross section, $\sim 10^{-56}$ $\text{cm}^4 \text{s}$, of Ne$^{8+}$ obtained within the perturbative nonrelativistic framework for monochromatic light [J. Phys. B {\bf 34}, 4857 (2001)] and the experimental value, $7 \times 10^{-54}$ $\text{cm}^4 \text{s}$, reported in [Phys. Rev. Lett. {\bf 106}, 083002 (2011)] at a photon energy of 1110 eV. To this end, we consider Ne$^{8+}$ exposed to deterministic and chaotic ensembles of intense x-ray pulses. The time-dependent configuration-interaction singles (TDCIS) method is used to quantitatively describe nonlinear ionization of Ne$^{8+}$ induced by coherent intense ultrashort x-ray laser pulses. The impact of the bandwidth of a chaotic ensemble of x-ray pulses on the effective two-photon ionization cross section is studied within the lowest nonvanishing order of perturbation theory. We find that, at a bandwidth of 11 eV, the effective two-photon ionization cross section of Ne$^{8+}$ at a photon energy of 1110 eV amounts to $5 \times 10^{-57}$ and $1.6 \times 10^{-55}$ $\text{cm}^4 \text{s}$ for a deterministic ensemble and a chaotic ensemble, respectively. We show that the enhancement obtained for a chaotic ensemble of pulses originates from the presence of the one-photon 1$s^2$--1$s4p$ resonance located at 1127 eV. Using the TDCIS approach, we also show that, for currently available radiation intensities, two-photon ionization of a 1$s$ electron in neutral neon remains less probable than one-photon ionization of a valence electron.

physics.atom-ph↗

The Impact of Multichannel and Multipole Effects on the Cooper Minimum in the High-Harmonics Spectrum of Argon

We investigate the relevance of multiple-orbital and multipole effects during high-harmonic generation (HHG). The time-dependent configuration-interaction singles (TDCIS) approach is used to study the impact of the detailed description of the residual electron-ion interaction on the HHG spectrum. We find that the shape and position of the Cooper minimum in the HHG spectrum of argon changes significantly whether or not interchannel interactions are taken into account. The HHG yield can be underestimated by up to 2 orders of magnitude in the energy regio of 30-50 eV. We show that the argument of low ionization probability is not sufficient to justify ignoring multiple-orbital contributions. Additionally, we find the HHG yield is sensitive to the nonspherical multipole character of the electron-ion interaction.

physics.atom-ph↗

Decoherence in Attosecond Photoionization

The creation of superpositions of hole states via single-photon ionization using attosecond extreme-ultraviolet pulses is studied with the time-dependent configuration interaction singles (TDCIS) method. Specifically, the degree of coherence between hole states in atomic xenon is investigated. We find that interchannel coupling not only affects the hole populations, it also enhances the entanglement between the photoelectron and the remaining ion, thereby reducing the coherence within the ion. As a consequence, even if the spectral bandwidth of the ionizing pulse exceeds the energy splittings among the hole states involved, perfectly coherent hole wave packets cannot be formed. For sufficiently large spectral bandwidth, the coherence can only be increased by increasing the mean photon energy.

physics.atom-ph↗

Alignment of asymmetric-top molecules using multiple-pulse trains

We theoretically analyze the effectiveness of multiple-pulse laser alignment methods for asymmetric-top molecules. As an example, we choose SO_2 and investigate the alignment dynamics induced by two different sequences, each consisting of four identical laser pulses. Each sequence differs only in the time delay between the pulses. Equally spaced pulses matching the alignment revival of the symmetrized SO_2 rotor model are exploited in the first sequence. The pulse separations in the second sequence are short compared to the rotation dynamics of the molecule and monotonically increase the degree of alignment until the maximum alignment is reached. We point out the significant differences between the alignment dynamics of SO_2 treated as an asymmetric-top and a symmetric-top rotor, respectively. We also explain why the fast sequence of laser pulses creates considerably stronger one-dimensional molecular alignment for asymmetric-top molecules. In addition, we show that multiple-pulse trains with elliptically polarized pulses do not enhance one-dimensional alignment or create three-dimensional alignment.

physics.atom-ph↗

Computational studies of x-ray scattering from three-dimensionally-aligned asymmetric-top molecules

We theoretically and numerically analyze x-ray scattering from asymmetric-top molecules three-dimensionally aligned using elliptically polarized laser light. A rigid-rotor model is assumed. The principal axes of the polarizability tensor are assumed to coincide with the principal axes of the moment of inertia tensor. Several symmetries in the Hamiltonian are identified and exploited to enhance the efficiency of solving the time-dependent Schrödinger equation for each rotational state initially populated in a thermal ensemble. Using a phase-retrieval algorithm, the feasibility of structure reconstruction from a quasi-adiabatically-aligned sample is illustrated for the organic molecule naphthalene. The spatial resolution achievable strongly depends on the laser parameters, the initial rotational temperature, and the x-ray pulse duration. We demonstrate that for a laser peak intensity of 5 TW/cm^2, a laser pulse duration of 100 ps, a rotational temperature of 10 mK, and an x-ray pulse duration of 1 ps, the molecular structure may be probed at a resolution of 1 Å.

physics.atom-ph↗