Generation of Large Vortex-Free Superfluid Helium Nanodroplets.

Superfluid helium nanodroplets are an ideal environment for the formation of metastable, self-organized dopant nanostructures. However, the presence of vortices often hinders their formation. Here, we demonstrate the generation of vortex-free helium nanodroplets and explore the size range in which they can be produced. From x-ray diffraction images of xenon-doped droplets, we identify that single compact structures, assigned to vortex-free aggregation, prevail up to 10^{8} atoms per droplet. This finding builds the basis for exploring the assembly of far-from-equilibrium nanostructures at low temperatures.

Ionization potentials of MgN (N = 7-56) clusters formed by spontaneous collapse of magnesium foam in helium nanodroplets.

The ionization potentials of magnesium clusters (MgN, N = 7-56) are determined by doping ultracold helium nanodroplets (HeM, M ≈ 52 000) with Mg atoms. Inspecting the particle size distributions resulting from non-resonant, short-wavelength, single-photon ionization gives evidence that beyond a certain ensemble size, the developing foam structure undergoes a spontaneous collapse on the way to the laser interaction region. As a result, hot Mg clusters form in the relaxation process. The spontaneous collapse manifests in a substantial change in the size distributions, when recording mass spectra at wavelengths shorter than 272 nm. Tracing individual MgN signals as a function of laser photon energy allows extraction of size-specific ionization potentials, which for small clusters show a good agreement with results obtained from density functional theory simulations. The further development is compared to calculations based on the liquid drop model. However, even when quantum effects are included, the simple scaling law is not able to reproduce the development of the ionization potentials. The results suggest that small neutral magnesium clusters behave as non-metallic. The comparison to electron affinities and band gaps obtained from photoemission experiments on MgN- provides information on the charge state dependence of the non-metal-to-metal transition and properties like the Mulliken electron negativity.

Phase-of-the-Phase Electron Momentum Spectroscopy on Single Metal Atoms in Helium Nanodroplets.

Magnesium atoms fully embedded in helium nanodroplets are exposed to two-color laser pulses, which trigger multiphoton above-threshold ionization (ATI). This allows exemplary study of the contribution of a dense, neutral, and finite medium on single electron propagation. The angular-resolved photoelectron spectra show striking differences with respect to results obtained on free atoms. Scattering of the individual Mg photoelectrons, when traversing the neutral helium environment, causes the angular distribution to become almost isotropic. Furthermore, the appearance of higher-energy electrons is observed, indicating the impact of the droplet on the concerted emission process. Phase-of-the-phase spectroscopy, however, reveals a marked loss in the 2ω-ω phase dependence of the electron signal. Taking into account sideband formation on a quantitative level, a Monte Carlo simulation which includes laser-assisted electron scattering can reproduce the experimental spectra and give insights into the strong-field-induced electron emission from disordered systems.

Photoelectron Spectroscopy on Magnesium Ensembles in Helium Nanodroplets.

The electronic properties of magnesium embedded in helium nanodroplets are investigated as a function of the doping level by combining resonant two-photon ionization with photoelectron spectroscopy. Photon absorption near the atomic 31P1 ← 31S0 transition triggers the dynamics, which is probed on a nanosecond timescale by the subsequent absorption of the ionizing photon. Striking similarities in the photoelectron spectra for different doping levels and the population of atomic states well beyond 31P1 evidence an energy release process being relevant for a wide range of droplet sizes and doping conditions. From the statistical analysis, one can infer that instead of a single compact cluster size, a loosely bound Mg atom ensemble is responsible for the resulting spectra.

Comparison of Electron and Ion Emission from Xenon Cluster-Induced Ignition of Helium Nanodroplets.

The charging dynamics of helium droplets driven by embedded xenon cluster ignition in strong laser fields is studied by comparing the abundances of helium and highly charged Xe ions to the electron signal. Femtosecond pump-probe experiments show that near the optimal delay for highly charged xenon the electron yield increases, especially at low energies. The electron signature can be traced back to the ionization of the helium environment by Xe seed electrons. Accompanying molecular dynamics simulations suggest a two-step ionization scenario in the Xe-He core-shell system. In contrast to xenon, the experimental signal of the helium ions, as well as low-energy electron emission show a deviating delay dependence, indicating differences in the temporal and spacial development of the charge state distribution of Xe core and He surrounding. From the pump-probe dependence of the electron emission, effective temperatures can be extracted, indicating the nanoplasma decay.

Publisher Correction: Nanoplasmonic electron acceleration by attosecond-controlled forward rescattering in silver clusters.

The original PDF version of this Article contained an error in Equation 1. The original HTML version of this Article contained errors in Equation 2 and Equation 4. These errors have now been corrected in both the PDF and the HTML versions of the Article.

Nanoplasmonic electron acceleration by attosecond-controlled forward rescattering in silver clusters.

In the strong-field photoemission from atoms, molecules, and surfaces, the fastest electrons emerge from tunneling and subsequent field-driven recollision, followed by elastic backscattering. This rescattering picture is central to attosecond science and enables control of the electron's trajectory via the sub-cycle evolution of the laser electric field. Here we reveal a so far unexplored route for waveform-controlled electron acceleration emerging from forward rescattering in resonant plasmonic systems. We studied plasmon-enhanced photoemission from silver clusters and found that the directional acceleration can be controlled up to high kinetic energy with the relative phase of a two-color laser field. Our analysis reveals that the cluster's plasmonic near-field establishes a sub-cycle directional gate that enables the selective acceleration. The identified generic mechanism offers robust attosecond control of the electron acceleration at plasmonic nanostructures, opening perspectives for laser-based sources of attosecond electron pulses.

Efficient laser-driven proton acceleration from cylindrical and planar cryogenic hydrogen jets.

We report on recent experimental results deploying a continuous cryogenic hydrogen jet as a debris-free, renewable laser-driven source of pure proton beams generated at the 150 TW ultrashort pulse laser Draco. Efficient proton acceleration reaching cut-off energies of up to 20 MeV with particle numbers exceeding 109 particles per MeV per steradian is demonstrated, showing for the first time that the acceleration performance is comparable to solid foil targets with thicknesses in the micrometer range. Two different target geometries are presented and their proton beam deliverance characterized: cylindrical (∅ 5 µm) and planar (20 µm × 2 µm). In both cases typical Target Normal Sheath Acceleration emission patterns with exponential proton energy spectra are detected. Significantly higher proton numbers in laser-forward direction are observed when deploying the planar jet as compared to the cylindrical jet case. This is confirmed by two-dimensional Particle-in-Cell (2D3V PIC) simulations, which demonstrate that the planar jet proves favorable as its geometry leads to more optimized acceleration conditions.

Particulate matter from both heavy fuel oil and diesel fuel shipping emissions show strong biological effects on human lung cells at realistic and comparable in vitro exposure conditions.

BACKGROUND: Ship engine emissions are important with regard to lung and cardiovascular diseases especially in coastal regions worldwide. Known cellular responses to combustion particles include oxidative stress and inflammatory signalling. OBJECTIVES: To provide a molecular link between the chemical and physical characteristics of ship emission particles and the cellular responses they elicit and to identify potentially harmful fractions in shipping emission aerosols. METHODS: Through an air-liquid interface exposure system, we exposed human lung cells under realistic in vitro conditions to exhaust fumes from a ship engine running on either common heavy fuel oil (HFO) or cleaner-burning diesel fuel (DF). Advanced chemical analyses of the exhaust aerosols were combined with transcriptional, proteomic and metabolomic profiling including isotope labelling methods to characterise the lung cell responses. RESULTS: The HFO emissions contained high concentrations of toxic compounds such as metals and polycyclic aromatic hydrocarbon, and were higher in particle mass. These compounds were lower in DF emissions, which in turn had higher concentrations of elemental carbon ("soot"). Common cellular reactions included cellular stress responses and endocytosis. Reactions to HFO emissions were dominated by oxidative stress and inflammatory responses, whereas DF emissions induced generally a broader biological response than HFO emissions and affected essential cellular pathways such as energy metabolism, protein synthesis, and chromatin modification. CONCLUSIONS: Despite a lower content of known toxic compounds, combustion particles from the clean shipping fuel DF influenced several essential pathways of lung cell metabolism more strongly than particles from the unrefined fuel HFO. This might be attributable to a higher soot content in DF. Thus the role of diesel soot, which is a known carcinogen in acute air pollution-induced health effects should be further investigated. For the use of HFO and DF we recommend a reduction of carbonaceous soot in the ship emissions by implementation of filtration devices.

Formation of coherent rotational wavepackets in small molecule-helium clusters using impulsive alignment.

We show that rotational line spectra of molecular clusters with near zero permanent dipole moments can be observed using impulsive alignment. Aligned rotational wavepackets were generated by non-resonant interaction with intense femtosecond laser pump pulses and then probed using Coulomb explosion by a second, time-delayed femtosecond laser pulse. By means of a Fourier transform a rich spectrum of rotational eigenstates was derived. For the smallest cluster, C(2)H(2)-He, we were able to establish essentially all rotational eigenstates up to the dissociation threshold on the basis of theoretical level predictions. The C(2)H(2)-He complex is found to exhibit distinct features of large amplitude motion and very early onset of free internal rotor energy level structure.

Formation and properties of metal clusters isolated in helium droplets.

The unique conditions forming atomic and molecular complexes and clusters using superfluid helium nanodroplets have opened up an innovative route for studying the physical and chemical properties of matter on the nanoscale. This review summarizes the specific characteristics of the formation of atomic clusters partly generated far from equilibrium in the helium environment. Special emphasis is on the optical response, electronic properties as well as dynamical processes which are mostly affected by the surrounding quantum matrix. Experiments include the optical induced response of isolated cluster systems in helium under quite different excitation conditions ranging from the linear regime up to the violent interaction with a strong laser field leading to Coulomb explosion and the generation of highly charged atomic fragments. The variety of results on the outstanding properties in the quantum size regime highlights the peculiar capabilities of helium nanodroplet isolation spectroscopy.

Ion induced snowballs as a diagnostic tool to investigate the caging of metal clusters in large helium droplets.

Metal clusters embedded in ultracold helium nanodroplets are exposed to femtosecond laser pulses with intensities of 10(13)-10(14) W/cm2. The influence of the matrix on the ionization and fragmentation dynamics is studied by pump-probe time-of-flight mass spectrometry. Special attention is paid to the generation of helium snowballs around positive metal ions (Me(z+)He(N), z=1,2). Closings of the first and second helium shells are found for silver at N(1)=10,12 and N(2)=32,44, as well as for magnesium at N1=19-20. The distinct abundance enhancement of helium snowballs in the presence of isolated atoms and small clusters in the droplets is used as a diagnostics to explore the cage effect. For silver, a reaggregation of the clusters is observed at 30 ps after femtosecond laser excitation.

Photoelectron studies of neutral Ag3 in helium droplets.

Photoelectron spectra of neutral silver trimers, grown in ultracold helium nanodroplets, are recorded after ionization with laser pulses via a strong optical resonance of this species. Varying the photon energy reveals that direct vertical two-photon ionization is hindered by a rapid relaxation into the lower edge of a long-living excited state manifold. An analysis of the ionization threshold of the embedded trimer yields an ionization potential of 5.74+/-0.09 eV consistent with the value found in the gas phase. The asymmetrical form of the electron energy spectrum, which is broadened toward lower kinetic energies, is attributed to the influence of the matrix on the photoionization process. The lifetime of the excited state was measured in a two-color pump-probe experiment to be 5.7+/-0.6 ns.

Excited-state relaxation of Ag8 clusters embedded in helium droplets.

Neutral silver clusters Ag(N) are grown in ultracold helium nanodroplets. By exploiting a strong absorption resonance recently found for Ag8, first photoelectron spectra of this neutral species are recorded. Variation of the laser photon energy reveals that direct vertical two-photon ionization is hindered by rapid relaxation into the lower edge of a long-living excited state manifold. The analysis of the dynamics gives a precise value of (6.89+/-0.09) eV for the vertical ionization potential of Ag8. The influence of the helium matrix on photoemission is discussed.