Optimal photoelectron circular dichroism of a model chiral system.

We optimize the internuclear geometry and electronic structure of a model chiral system to achieve a maximal photoelectron circular dichroism (PECD) in its one-photon ionization by circularly polarized light. The electronic structure calculations are performed by the single center method, while the optimization is done using quantum alchemy employing a Taylor series expansion. Thereby, the effect of bond lengths and uncompensated charge distributions on the chiral response of the model is investigated theoretically in some detail.

Photoelectron Circular Dichroism in the Spin-Polarized Spectra of Chiral Molecules.

We studied strong-field multiphoton ionization of 1-iodo-2-methylbutane enantiomers with 395 nm circularly polarized laser pulses experimentally and theoretically. For randomly oriented molecules, we observe spin polarization up to about 15%, which is independent of the molecular enantiomer. Our experimental findings are explained theoretically as an intricate interplay between three contributions from HOMO, HOMO-1, and HOMO-2, which are formed of 5p-electrons of the iodine atom.

Theoretical study of spin polarization in multiphoton ionization of Xe.

Spin polarization in the multiphoton above-threshold ionization of 5p3/2- and 5p1/2-electrons of Xe with intense 395nm, circularly polarized laser pulses, is investigated theoretically. For this purpose, we solve the time-dependent Schrödinger equation on the basis of spherical spinors. We, thus, simultaneously propagate the spin-up and spin-down single-active-electron wave packets, driven by the laser pulses in the ionic potential, which includes the spin-orbit interaction explicitly.

Electron Dynamics and Correlations During High-Order Harmonic Generation in Be.

We investigate theoretically the high-order harmonic generation in beryllium atom irradiated by a short 1850 nm linearly polarized laser pulse in the intermediate strong-field ionization regime with the Keldysh parameter of 0.85. To this end, the respective time-dependent Schrödinger equation is solved by the time-dependent restricted-active-space configuration-interaction (TD-RASCI) method.

Photoelectron circular dichroism in the multiphoton ionization by short laser pulses. III. Photoionization of fenchone in different regimes.

Photoelectron circular dichroism (PECD) in different regimes of multiphoton ionization of fenchone is studied theoretically using the time-dependent single center method. In particular, we investigate the chiral response to the one-color multiphoton or strong-field ionization by circularly polarized 400 nm and 814 nm optical laser pulses or 1850 nm infrared pulse. In addition, the broadband ionization by short coherent circularly polarized 413-1240 nm spanning pulse is considered.

Recoil-Induced Asymmetry of Nondipole Molecular Frame Photoelectron Angular Distributions in the Hard X-ray Regime.

We investigate angular emission distributions of the 1s photoelectrons of N_{2} ionized by linearly polarized synchrotron radiation at hν=40  keV. As expected, nondipole contributions cause a very strong forward-backward asymmetry in the measured emission distributions. In addition, we observe an unexpected asymmetry with respect to the polarization direction, which depends on the direction of the molecular fragmentation.

Controlling Dynamics of Postcollision Interaction.

A general scheme to get insight and to control postcollision interaction (PCI) by means of sequential double ionization with two high-frequency pulses is discussed. In particular, we propose to consider PCI of a slow photoelectron released by the pump pulse from a neutral atom with a fast photoelectron released by the time-delayed probe pulse from the created ion. This scheme is exemplified by the ab initio calculations performed for the prototypical helium atom.

Photoelectron Circular Dichroism with Two Overlapping Laser Pulses of Carrier Frequencies ω and 2ω Linearly Polarized in Two Mutually Orthogonal Directions.

Using a model methanelike chiral system, we theoretically demonstrate a possibility to access photoelectron circular dichroism (PECD) by a single experiment with two overlapping laser pulses of carrier frequencies ω and 2ω, which are linearly polarized in two mutually orthogonal directions. Depending on the relative phase, the resulting electric field can be tailored to have two different rotational directions in the upper and lower hemispheres along the polarization of the ω pulse. We predict a strong forward-backward asymmetry in the emission of photoelectrons from randomly oriented samples, which has an opposite sign in the upper and lower hemispheres.

Circular Dichroism in Fluorescence Emission Following the C 1s→π* Excitation and Resonant Auger Decay of Carbon Monoxide.

Dichroism in angle-resolved spectra of circularly polarized fluorescence from freely-rotating CO molecules was studied experimentally and theoretically. For this purpose, carbon monoxide in the gas phase was exposed to circularly polarized soft X-ray synchrotron radiation. The photon energy was tuned across the C 1s→π* resonant excitation, which decayed via the participator Auger transition into the CO⁺ A ²Π state.

Quantum Electrodynamical Corrections to Energy Levels of Diatomic Quasimolecules.

We elaborate an ab initio approach for the evaluation of the one-loop quantum electrodynamical corrections to energy levels of diatomic quasimolecules. The approach accounts for the interaction between an electron and two nuclei in all orders in Zα and can be applied for a wide range of internuclear distances, up to R≈1000  fm. Based on the developed theory, detailed calculations are performed for the self-energy and vacuum-polarization corrections to the energy of the 1σ(g) ground state of the U(92+)-U(91+) dimer that can be produced in slow ion-ion collisions.

Photoelectron circular dichroism in the multiphoton ionization by short laser pulses. I. Propagation of single-active-electron wave packets in chiral pseudo-potentials.

A theoretical method to study the angle-resolved multiphoton ionization of polyatomic molecules is developed. It is based on the time-dependent formulation of the Single Center (TDSC) method and consists in the propagation of single-active-electron wave packets in the effective molecular potentials in the presence of intense laser pulses. For this purpose, the time-dependent Schrödinger equation for one electron, moving in a molecular field and interacting with an arbitrary laser pulse, is solved in spherical coordinates by an efficient numerical approach.

Hartree-Fock calculation of the differential photoionization cross sections of small Li clusters.

Cross sections and angular distribution parameters for the single-photon ionization of all electron orbitals of Li2-8 are systematically computed in a broad interval of the photoelectron kinetic energies for the energetically most stable geometry of each cluster. Calculations of the partial photoelectron continuum waves in clusters are carried out by the single center method within the Hartree-Fock approximation. We study photoionization cross sections per one electron and analyze in some details general trends in the photoionization of inner and outer shells with respect to the size and geometry of a cluster.

Young-type interference in projectile-electron loss in energetic ion-molecule collisions.

Under certain conditions an electron bound in a fast projectile ion, colliding with a molecule, interacts mainly with the nuclei and inner shell electrons of atoms forming the molecule. Because of their compact localization in space and distinct separation from each other, these molecular centers play in such collisions a role similar to that of optical slits in light scattering leading to pronounced interference in the spectra of the electron emitted from the projectile.

Exploring relativistic many-body recoil effects in highly charged ions.

The relativistic recoil effect has been the object of experimental investigations using highly charged ions at the Heidelberg electron beam ion trap. Its scaling with the nuclear charge Z boosts its contribution to a measurable level in the magnetic-dipole (M1) transitions of B- and Be-like Ar ions. The isotope shifts of 36Ar versus 40Ar have been detected with sub-ppm accuracy, and the recoil effect contribution was extracted from the 1s(2)2s(2)2p 2P(1/2) - 2P(3/2) transition in Ar13+ and the 1s(2)2s2p 3P1-3P2 transition in Ar14+.

A finite B-spline basis set for accurate diatomic molecule calculations.

A finite basis set particularly adapted for solving the Hartree-Fock equation for diatomic molecules in prolate spheroidal coordinates has been constructed. These basis functions have been devised as products of B-splines times associated Legendre polynomials. Due to the large number of B-splines, the resulting set of eigenfunctions is amply distributed over excited states.

Towards a test of QED in investigations of the hyperfine splitting in heavy ions.

A possibility for investigations of quantum electrodynamics (QED) in experiments on the hyperfine splitting in heavy ions is examined. It is found that QED effects can be probed on the level of a few percent in a specific difference of the hyperfine splitting values in hydrogenlike and lithiumlike bismuth. This could provide a test of QED in the strongest electric field available at present for experimental study.

Two-photon exchange corrections to the 2p(1/2)-2s transition energy in Li-like high- Z ions.

A rigorous QED calculation of the two-photon exchange corrections to the 2p(1/2)- 2s transition energy in Li-like high- Z ions is presented. The contribution due to an exchange by more than two photons is evaluated within the Breit approximation. The resulting theoretical value of the 2p(1/2)- 2s transition energy in Li-like uranium is found to be 280.