A significant fraction of superfluid helium nanodroplets produced in a free-jet expansion has been observed to gain high angular momentum resulting in large centrifugal deformation. We measured single-shot diffraction patterns of individual rotating helium nanodroplets up to large scattering angles using intense extreme ultraviolet light pulses from the FERMI free-electron laser. Distinct asymmetric features in the wide-angle diffraction patterns enable the unique and systematic identification of the three-dimensional droplet shapes. The analysis of a large data set allows us to follow the evolution from axisymmetric oblate to triaxial prolate and two-lobed droplets. We find that the shapes of spinning superfluid helium droplets exhibit the same stages as classical rotating droplets while the previously reported metastable, oblate shapes of quantum droplets are not observed. Our three-dimensional analysis represents a valuable landmark for clarifying the interrelation between morphology and superfluidity on the nanometer scale.

Spin and orbital magnetic moments of cationic iron, cobalt, and nickel clusters have been determined from x-ray magnetic circular dichroism spectroscopy. In the size regime of n = 10 − 15 atoms, these clusters show strong ferromagnetism with maximized spin magnetic moments of 1 µB per empty 3d state because of completely filled 3d majority spin bands. The only exception is Fewhere an unusually low average spin magnetic moment of 0.73 ± 0.12 µB per unoccupied 3d state is detected; an effect, which is neither observed for Co + 13 nor Ni + 13 . This distinct behavior can be linked to the existence and accessibility of antiferromagnetic, paramagnetic, or nonmagnetic phases in the respective bulk phase diagrams of iron, cobalt, and nickel. Compared to the experimental data, available density functional theory calculations generally seem to underestimate the spin magnetic moments significantly. In all clusters investigated, the orbital magnetic moment is quenched to 5 − 25 % of the atomic value by the reduced symmetry of the crystal field. The magnetic anisotropy energy is well below 65 µeV per atom.

Coherent diffractive imaging of individual free nanoparticles has opened routes for the in situ analysis of their transient structural, optical, and electronic properties. So far, single-shot single-particle diffraction was assumed to be feasible only at extreme ultraviolet and X-ray free-electron lasers, restricting this research field to large-scale facilities. Here we demonstrate single-shot imaging of isolated helium nanodroplets using extreme ultraviolet pulses from a femtosecond-laser-driven high harmonic source. We obtain bright wide-angle scattering patterns, that allow us to uniquely identify hitherto unresolved prolate shapes of superfluid helium droplets. Our results mark the advent of single-shot gas-phase nanoscopy with lab-based short-wavelength pulses and pave the way to ultrafast coherent diffractive imaging with phase-controlled multicolor fields and attosecond pulses.

The magnetic moment of a single impurity atom in a finite free electron gas is studied in a combined x-ray magnetic circular dichroism spectroscopy, charge transfer multiplet calculation, and density functional theory study of size-selected free chromium-doped gold clusters. The observed size dependence of the local magnetic moment can be understood as a transition from a local moment to a mixed valence regime. This shows that the Anderson impurity model essentially describes finite systems even though the discrete density of states introduces a significant deviation from a bulk metal, and the free electron gas is only formed by less than 10 electrons. Electronic shell closure in the gold host minimizes the interaction of localized impurity states with the confined free electron gas and preserves the magnetic moment of 5 μ_{B} fully in CrAu_{2}^{+} and almost fully in CrAu_{6}^{+}. Even for open-shell species, large local moments are observed that scale with the energy gap of the gold cluster. This indicates that an energy gap in the free electron gas stabilizes the local magnetic moment of the impurity atom.