Resolving in time the dynamics of light absorption by atoms and molecules, and the electronic rearrangement this induces, is among the most challenging goals of attosecond spectroscopy. The attoclock is an elegant approach to this problem, which encodes ionization times in the strongfield regime. However, the accurate reconstruction of these times from experimental data presents a formidable theoretical challenge. Here, we solve this problem by combining analytical theory with ab-initio numerical simulations. We apply our theory to numerical attoclock experiments on the hydrogen atom to extract ionization time delays and analyse their nature. Strong field ionization is often viewed as optical tunnelling through the barrier created by the field and the core potential. We show that, in the hydrogen atom, optical tunnelling is instantaneous. By calibrating the attoclock using the hydrogen atom, our method opens the way to identify possible delays associated with multielectron dynamics during strong-field ionization.

We present experimental measurements and theoretical calculations of photoionization time delays from the 3s and 3p shells in Ar in the photon energy range of 32-42 eV. The experimental measurements are performed by interferometry using attosecond pulse trains and the infrared laser used for their generation. The theoretical approach includes intershell correlation effects between the 3s and 3p shells within the framework of the random phase approximation with exchange (RPAE). The connection between single-photon ionization and the two-color two-photon ionization process used in the measurement is established using the recently developed asymptotic approximation for the complex transition amplitudes of laser-assisted photoionization. We compare and discuss the theoretical and experimental results especially in the region where strong intershell correlations in the 3s → kp channel lead to an induced "Cooper" minimum in the 3s ionization cross-section.

We analyze the time delay between emission of photoelectrons from the outer valence ns and np subshells in noble gas atoms following absorption of an attosecond extreme ultraviolet pulse. Various processes such as elastic scattering of the photoelectron on the parent ion and many-electron correlation affect the apparent "time zero" when the photoelectron leaves the atom. This qualitatively explains the time delay between photoemission from the 2s and 2p subshells of Ne as determined experimentally by attosecond streaking [Science 328, 1658 (2010)]. However, with our extensive numerical modeling, we were only able to account for less than half of the measured time delay of 21 ± 5 as. We argue that the extreme ultraviolet pulse alone cannot produce such a large time delay and it is the streaking IR field that is most likely responsible for this effect.

We use the non-relativistic random phase approximation with exchange to perform calculations of valence shell photoionization of Ne, Ar, Kr and Xe from their respective thresholds to photon energy of 200 eV. The energy derivative of the complex phase of the photoionization matrix elements is converted to the photoelectron group delay that can be measured in attosecond streaking or twophoton sideband interference experiments. Comparison with reported time delay measurements in Ne and Ar at a few selected photon energies is made. Systematic mapping of time delay across a wide range of photon energies in several atomic targets allows to highlight important aspects of fundamental atomic physics that can be probed by attosecond time delay measurements.