We present a first investigation of structural properties of Ag clusters with a diameter of up to 5.5 nm grown inside superfluid helium nanodroplets (He_N) and deposited on an amorphous C surface. With high resolution transmission electron microscope images we are able to show that in addition to the crystalline face centered cubic (fcc) structure, noncrystalline icosahedral (Ih), and decahedral (Dh) morphologies are grown. Relative abundances (56% fcc, 31% Dh, and 13% Ih) as well as the size distribution of each morphology (mean diameters ${\overline{d}}_{\mathrm{fcc}}=2.62\left(5\right)$ nm, ${\overline{d}}_{\mathrm{Dh}}=3.34\left(7\right)$ nm, and ${\overline{d}}_{\mathrm{Ih}}=3.93\left(2\right)$ nm) do not reflect the situation expected from pure energetic considerations, where small Ihs should be followed by medium sized Dhs and large fccs. Instead, kinetic factors seem to play an important role in the formation of these structures, as it appears to be the case for clusters formed by inert gas aggregation. Considering the low temperatures (0.37 K) and extremely high cooling rates, we discuss basic ideas that might lead to a qualitative picture of the cluster formation process inside He_N.

Superfluid helium nanodroplets provide a versatile substrate to cool atoms and molecules, and to assemble weakly bound complexes. Absence of spin-relaxation mechanisms makes He nanodroplets ideal to isolate open-shell atoms and create a spin-polarized system. Here, we show the first coherent manipulation of such a system by resonant excitation of a magnetic-dipole transition. Observation of $\approx 50$ Rabi oscillations demonstrates coherent population transfer with minimal dephasing. Ours is also the first application of ESR spectroscopy to doped He nanodroplets. This unique environment results in extremely sharp lines and hyperfine-resolved spectra: those of single ${}^{39}\mathrm{K}$ and ${}^{85}\mathrm{Rb}$ dopant atoms presented here denote an increase of the Fermi contact interaction, which we can follow as a function of droplet size, reflecting the distortion of the valence-electron wave function due to the surrounding He.

The observation of chemical reactions on the time scale of the motion of electrons and nuclei has been made possible by lasers with ever shortened pulse lengths. Superfluid helium represents a special solvent that permits the synthesis of novel classes of molecules that have eluded dynamical studies so far. However, photoexcitation inside this quantum solvent triggers a pronounced response of the solvation shell, which is not well understood. Here, we present a mechanistic description of the solvent response to photoexcitation of indium (In) dopant atoms inside helium nanodroplets (He_N), obtained from femtosecond pump–probe spectroscopy and time-dependent density functional theory simulations. For the In–He_N system, part of the excited state electronic energy leads to expansion of the solvation shell within 600 fs, initiating a collective shell oscillation with a period of about 30 ps. These coupled electronic and nuclear dynamics will be superimposed on intrinsic photoinduced processes of molecular systems inside helium droplets.

We present a series of molecular dynamics simulations on the surface deposition process of initially free silver clusters (Ag_n) with different sizes (n = 100–2000) and morphologies. During the whole deposition process the morphology of the clusters was studied as a function of the landing conditions. These conditions include variations of the depth and range of the substrate potential as well as the thermal coupling to the surface and a variation of the impact velocity of the free clusters. Depending on the applied conditions the clusters' final form ranges from spread out fragments via deformed and restructured heaps to quasi unchanged spherical clusters sitting at the surface. Under certain landing conditions larger clusters retain their initial multiply twinned morphology upon deposition, while smaller ones undergo structural transitions to form single domain particles. Furthermore, the occurrence of a structural transition depends on the initial structure—initially decahedral clusters tend to conserve their morphology better than icosahedral ones. The same behavior can also be observed in our experiments, where silver clusters were grown in helium nanodroplets and subsequently deposited on amorphous carbon substrates.