Unveiling the Inhomogeneous Nature of Strong Field Ionization in Extended Systems.

Intense light-induced fragmentation of spherical clusters produces highly energetic ions with characteristic spatial distributions. By subjecting argon clusters to a wavelength tunable laser, we show that ion emission energy and anisotropy can be controlled through the wavelength-isotropic and energetic for shorter wavelengths and increasingly anisotropic at longer wavelengths. The anisotropic part of the energy spectrum, consisting of multiply charged high-energy ions, is considerably more prominent at longer wavelengths. Classical molecular dynamics simulations reveal that cluster ionization occurs inhomogeneously producing a columnlike charge distribution along the laser polarization direction. This previously unknown distribution results from the dipole response of the neutral cluster which creates an enhanced field at the surface, preferentially triggering ionization at the poles. The subsequently formed nanoplasma provides an additional wavelength-dependent ionization mechanism through collisional ionization, efficiently homogenizing the system only at short wavelengths close to resonance. Our results open the door to studying polarization induced effects in nanostructures and complex molecules and provide a missing piece in our understanding of anisotropic ion emission.

Universal High-Energy Photoelectron Emission from Nanoclusters Beyond the Atomic Limit.

Rescattering by electrons on classical trajectories is central to understand photoelectron and high-harmonic emission from isolated atoms or molecules in intense laser pulses. By controlling the cluster size and the quiver amplitude of electrons, we demonstrate how rescattering influences the energy distribution of photoelectrons emitted from noble gas nanoclusters. Our experiments reveal a universal dependence of photoelectron energy distributions on the cluster size when scaled by the field driven electron excursion, establishing a unified rescattering picture for extended systems with the known atomic dynamics as the limit of zero extension. The result is supported by molecular dynamics calculations and rationalized with a one-dimensional classical model.

Prevailing features of x-ray-induced molecular electron spectra revealed with fullerenes.

X-ray photoabsorption from intense short pulses by a molecule triggers complicated electron and subsequently ion dynamics, leading to photoelectron spectra, which are difficult to interpret. Illuminating fullerenes offers a way to separate out the electron dynamics since the cage structure confines spatially the origin of photo- and Auger electrons. Together with the sequential nature of the photoprocesses at intensities available at x-ray free-electron lasers, this allows for a remarkably detailed interpretation of the photoelectron spectra, as we will demonstrate. The general features derived can serve as a paradigm for less well-defined situations in other large molecules or clusters.