We study photoionization of argon atoms excited by attosecond pulses using an interferometric measurement technique. We measure the difference in time delays between electrons emitted from the 3s(2) and from the 3p(6) shell, at different excitation energies ranging from 32 to 42 eV. The determination of photoemission time delays requires taking into account the measurement process, involving the interaction with a probing infrared field. This contribution can be estimated using a universal formula and is found to account for a substantial fraction of the measured delay.

We study the temporal aspects of laser-assisted extreme ultraviolet (XUV) photoionization using attosecond pulses of harmonic radiation. The aim of this paper is to establish the general form of the phase of the relevant transition amplitudes and to make the connection with the time-delays that have been recently measured in experiments. We find that the overall phase contains two distinct types of contributions: one is expressed in terms of the phase-shifts of the photoelectron continuum wavefunction while the other is linked to continuum-continuum transitions induced by the infrared (IR) laser probe. Our formalism applies to both kinds of measurements reported so far, namely the ones using attosecond pulse trains of XUV harmonics and the others based on the use of isolated attosecond pulses (streaking). The connection between the phases and the time-delays is established with the help of finite difference approximations to the energy derivatives of the phases. The observed time-delay is a sum of two components: a one-photon Wigner-like delay and an universal delay that originates from the probing process itself.

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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.

The optical spectra of hydrogen-passivated diamond clusters (diamondoids) precisely defined in size and shape have been measured in the gas phase, i.e., under an environment similar to boundary conditions typically assumed by theory. Characteristic optical properties evolve for these wide band-gap semiconductor nanocrystals as a function of size, shape, and symmetry in the subnanometer regime. These effects have not previously been theoretically predicted. The optical response of the tetrahedral-shaped C_{26}H_{32} diamond cluster [1(2,3)4] pentamantane is found to be remarkably similar to that of bulk diamond.