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 3s2 and from the 3p6 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 report the generation, compression, and delivery on target of ultrashort extreme-ultraviolet light pulses using external amplitude and phase control. Broadband harmonic radiation is first generated by focusing an infrared laser with a carefully chosen intensity into a gas cell containing argon atoms. The emitted light then goes through a hard aperture and a thin aluminum filter that selects a 30-eV bandwidth around a 30-eV photon energy and synchronizes all of the components, thereby enabling the formation of a train of almost Fourier-transform-limited single-cycle 170 attosecond pulses. Our experiment demonstrates a practical method for synthesizing and controlling attosecond waveforms.

We report experimental results on x-ray diffraction of quantum-state-selected and strongly aligned ensembles of the prototypical asymmetric rotor molecule 2,5-diiodobenzonitrile using the Linac Coherent Light Source. The experiments demonstrate first steps toward a new approach to diffractive imaging of distinct structures of individual, isolated gas-phase molecules. We confirm several key ingredients of single molecule diffraction experiments: the abilities to detect and count individual scattered x-ray photons in single shot diffraction data, to deliver state-selected, e.g., structural-isomer-selected, ensembles of molecules to the x-ray interaction volume, and to strongly align the scattering molecules. Our approach, using ultrashort x-ray pulses, is suitable to study ultrafast dynamics of isolated molecules.

We investigate the spectral and temporal structure of high harmonic emission from argon exposed to an infrared laser field and its second harmonic. For a wide range of generating conditions, trains of attosecond pulses with only one pulse per infrared cycle are generated. The synchronization necessary for producing such trains ensures that they have a stable pulse-to-pulse carrier envelope phase, unlike trains generated from one color fields, which have two pulses per cycle and a $\pi$ phase shift between consecutive pulses. Our experiment extends the generation of phase stabilized few cycle pulses to the extreme ultraviolet regime.

Acomplete quantum-mechanical description of matter and its interaction with the environment requires detailed knowledge of a number of complex parameters. In particular, information about the phase of wavefunctions is important for predicting the behaviour of atoms, molecules or larger systems. In optics, information about the evolution of the phase of light in time¹ and space² is obtained by interferometry. To obtain similar information for atoms and molecules, it is vital to develop analogous techniques. Here we present an interferometric method for determining the phase variation of electronic wave packets in momentum space, and demonstrate its applicability to the fundamental process of single-photon ionization. We use a sequence of extreme-ultraviolet attosecond pulses^3,4 to ionize argon atoms and an infrared laser field, which induces a momentum shear⁵ between consecutive electron wave packets. The interferograms that result from the interaction of these wave packets provide useful information about their phase. This technique opens a promising new avenue for reconstructing the wavefunctions^6,7 of atoms and molecules and for following the ultrafast dynamics of electronic wave packets.