Two-photon processes are atomic processes in which an atom interacts simultaneously with two photons. Such processes describe a wide range of phenomena, such as two-photon decay \nand elastic or inelastic scattering of photons. In recent years two-photon processes involving highly charged heavy ions have become an active area of research. Such studies do not only consider the total transition or scattering rates but also their angular and polarization dependence. To support such examinations in this thesis I present a theoretical framework to describe these properties in all two-photon processes with bound initial and final states \nand involving heavy H-like or He-like ions. I demonstrate how this framework can be used in some detailed studies of different two-photon processes. Specifically a detailed analysis of two-photon decay of H-like and He-like ions in strong external electromagnetic fields shows the importance of considering the effect of such fields for the physics of such systems. Furthermore I studied the elastic Rayleigh as well as inelastic Raman scattering by heavy H-like ions. I found a number of previously unobserved phenomena in the angular and polarization dependence of the scattering cross-sections that do not only allow to study interesting details of the electronic structure of the ion but might also be useful for the measurement of weak physical effects in such systems.
Two-photon processes are atomic processes in which an atom interacts simultaneously with two photons. Such processes describe a wide range of phenomena, such as two-photon decay \nand elastic or inelastic scattering of photons. In recent years two-photon processes involving highly charged heavy ions have become an active area of research. Such studies do not only consider the total transition or scattering rates but also their angular and polarization dependence. To support such examinations in this thesis I present a theoretical framework to describe these properties in all two-photon processes with bound initial and final states \nand involving heavy H-like or He-like ions. I demonstrate how this framework can be used in some detailed studies of different two-photon processes. Specifically a detailed analysis of two-photon decay of H-like and He-like ions in strong external electromagnetic fields shows the importance of considering the effect of such fields for the physics of such systems. Furthermore I studied the elastic Rayleigh as well as inelastic Raman scattering by heavy H-like ions. I found a number of previously unobserved phenomena in the angular and polarization dependence of the scattering cross-sections that do not only allow to study interesting details of the electronic structure of the ion but might also be useful for the measurement of weak physical effects in such systems.
The hyperfine levels for the ground state of hydrogen are normally connected by magnetic dipole transitions. However, for astrophysical applications, it may be that two-photon electric dipole processes are also important over cosmological distances. This thesis sets up a general mathematical formalism for the calculation of two-photon processes within the hyperfine structure of an atom with spin 1/2, and applies it to the ground state of hydrogen. Rates are calculated for both spontaneous emission and absorption of radiation. Due to an extraordinary degree of cancellation in the matrix elements, the rates turn out to be too small to have a significant impact on astrophysical processes involving the absorption and emission of radiation. The results are nevertheless important in reducing the uncertainty due to possible contributions from these processes. Other two-photon processes involving Raman scattering are also considered and the relevant cross sections calculated. The calculations of the decay rate, absorption coefficient and Raman scattering cross section are extended to heavier hydrogenic ions as a function of the nuclear charge Z, using an approximate interpolation formula for the hyperfine splitting in the ground state. Results are presented for the hydrogenlike ions from He+ to Pb81+. Modifications for the case of isotopes with a nuclear spin greater than 1/2 are briefly considered
Until recently, the nonlinear interaction between light and matter has been restricted to only low photon energies produced by optical lasers. However, about a decade ago, the rise of free-electron laser facilities revolutionized the field of nonlinear light-matter interaction by delivering intense high-energy light pulses. Today, such lasers are used for research in materials science, chemical technology, biophysical science, solid state physics as well as fundamental research. It is the new experimental possibilities provided by free-electron lasers that motivated the work presented in this thesis. Two-photon ionization process is one of the simplest nonlinear interactions in which absorption of two photons by an atom (or a molecule) leads to promoting one of its bound electrons to continuum. This work presents studies of two-photon ionization of neutral atoms. After a brief historical introduction to the topic of nonlinear light-matter interaction, the density matrix describing the state of an atom and a photoelectron following two-photon ionization is derived. In each successive chapter, part of this density matrix is used to obtain characteristic quantities such as total two-photon ionization cross section, photoelectron angular distributions, ion polarization or degree of polarization of fluorescence photon produced by subsequent decay of the photoion. Physical properties of these quantities are studied and intriguing phenomena, such as elliptical dichroism, polarization transfer as well as relativistic and screening effects are investigated.
In this thesis we investigate strong-field relativistic processes in highly charged ions. In the first part,we study resonance fluorescence of laser-driven highly charged ions in the relativistic regime by solving the time-dependent master equation in a multi-level model. Our ab initio approach based on the Dirac equation allows for investigating highly relativistic ions, and, consequently, provides a sensitive means to test correlated relativistic dynamics, bound-state quantum electrodynamic phenomena and nuclear effects by applying coherent light with x-ray frequencies. Atomic dipole or multipole moments may be determined to unprecedented accuracy by measuring the interference-narrowed fluorescence spectrum. Furthermore, we investigate the level structure of heavy hydrogenlike ions in laser beams. Interaction with the light field leads to dynamic shifts of the electronic energy levels, which is relevant for spectroscopic experiments. We apply a fully relativistic description of the electronic states by means of the Dirac equation. Our formalism goes beyond the dipole approximation and takes into account non-dipole effects of retardation and interaction with the magnetic field components of the laser beam. We predicted cross sections for the inter-shell trielectronic recombination (TR) and quadruelectronic recombination processes which have been experimentally confirmed in electron beam ion trap measurements, mainly for C-like ions, of Ar, Fe and Kr. For Kr30+, inter-shell TR contributions of nearly 6% to the total resonant photorecombination rate were found.
The inelastic Raman scattering of light by hydrogenlike ions has been studied by means of second-order perturbation theory and the relativistic Coulomb Green's-function approach. In particular, we investigate the total and angle-differential Raman cross sections as well as the magnetic sublevel population of the residual (excited) ions. Detailed calculations are performed for the inelastic scattering of photons by neutral hydrogen as well as hydrogenlike xenon and uranium ions, accompanied by the $1{s}_{1/2}\ensuremath{\rightarrow}2{s}_{1/2}$, $1{s}_{1/2}\ensuremath{\rightarrow}2{p}_{1/2}$, and $1{s}_{1/2}\ensuremath{\rightarrow}2{p}_{3/2}$ transitions. Moreover, we discuss how the Raman scattering is affected by relativistic and resonance effects as well as the higher-multipole contributions to the electron-photon interaction.
One active topic in Atomic Physics is the study of highly charged ions (HCI). These physical systems have a strong Coulomb field that provides a unique opportunity to investigate and validate relativistic, Quantum ElectroDynamics (QED), and many-body e ects. Moreover, fundamental test on symmetries and parity violation gives clues to the physics beyond the Standard Model. Thus, nowadays, a primary goal of Atomic Physics is the existence of precise experimental data and accurate theoretical calculations for these systems. In this thesis I focus on the investigation of forbidden radiative transitions in HCI. The main emphasis of this work is on atomic transitions, in which the selection rules forbids the emission of electric dipole photons. In this special type of radiative transition, the electron decays mainly through the emission of a single magnetic dipole photon, or two electric dipole photons. Both types of decay are investigated either experimentally or theoretically. The two-photon decay is only theoretically investigated, using a full relativistic formalism,in HCI with one or two electrons. Several physical e ects in the two photon decay, such as resonances, the Dirac’s negative continuum or angular correlations are considered. Related with the decay, two-photon excitation is also investigated. According to these evaluations, I stress the importance of relativistic and nondipolar e ects. Moreover, a new approach based on the B-polynomials basis set is employed on two-photon transitions. The second part of the work is devoted to the precise measurement of transitions in highly charged Ar with two to four electrons. For that matter, I describe the technical features of a double crystal spectrometer used to perform those measurements in HCI for the first time. This kind of spectrometer is able to perform absolute and precise measurements with an accuracy never achieved in these systems, which enables a comparison with recent QED calculations. I describe a Monte-Carlo code developed with the purpose of studying several systematic errors, as well as testing the various methods of retrieving physical quantities from raw data. Finally, I present the first absolute 2 ppm measurements on HCI with this spectrometer, paying special attention on the forbidden magnetic dipole transition in He-like Ar.
The two-photon decay of highly charged hydrogenlike ions is studied within the framework of second-order perturbation theory, based on Dirac's equation. Attention has been paid to the angle-angle correlations between the two emitted photons. In particular, the density matrix theory is applied in order to explore how these angle-angle correlations are affected by the alignment of the excited states of the ions. Detailed computations have been carried out for the $3{d}_{5∕2}\ensuremath{\rightarrow}1{s}_{1∕2}$ transition in hydrogenlike uranium U91+ ions for different (degrees of) initial alignment. It is shown that the angular correlation function is very sensitive to the alignment of the 3d5∕2 state, an effect which has to be accounted for in the analysis of all (future) two-photon decay experiments, for which the excited state of the ions is produced by relativistic ion-atom collisions.