<p>This dissertation discusses theoretical methods for describing photoionization in different systems in the context of time-dependent and time-independent non-relativistic and time-independent relativistic systems. We introduce a multichannel quantum defect theory (MQDT) model for describing photoionization in the context of pump-probe experiments. The basics of MQDT are introduced and specialized to the argon atom. Two energy regimes are studied in detail and compared to the experiment: (i) a perturbative calculation describing the dynamics of an autoionizing wave packet, (ii) a time-resolved calculation describing the two-photon ionization of a deeply bound wave packet. In both cases, the model accurately describes the relative ionization with respect to the two spin-orbit split thresholds of the ion and the oscillations shown in the delay between the pump and probe. We finalize with a brief presentation, which is primarily pedagogical, of how to use MQDT inside a finite box.</p> <p>Next, we use MQDT to describe the ytterbium atom in different energy regimes and varying degrees of approximation. The motivation behind this lies in the context of quantum information science, but our study is only concerned with calculating atomic properties. We start with a minimal MQDT model to describe the data observed in the experiment, followed by the presentation of an ab initio two-electron model. Both models compare very well to the experiment, and the ab initio method compares favorably with older spectroscopic results. In addition, we show unpublished results that incorporate the hyper-fine effects into the approximate model.</p> <p>Finally, we present an implementation of the two-electron variational R-matrix method for the Dirac equation, including the complete derivation of the solution of the Dirac equation in a central potential. We provide explicit analytic forms for the solutions of the Coulomb potential and use them to derive the generalized quantum defect parameters. A discussion of the variational R-matrix method for the Dirac equation in single and multichannel contexts is presented, with sample calculations for the beryllium and radium atoms. A chapter that summarizes and points to future work for each one of the projects concludes the work.</p>