Revisiting Thomson's model with multiply charged superfluid helium nanodroplets.

We study superfluid helium droplets multiply charged with Na+ or Ca+ ions. When stable, the charges are found to reside in equilibrium close to the droplet surface, thus representing a physical realization of Thomson's model. We find the minimum radius of the helium droplet that can host a given number of ions using a model whose physical ingredients are the solvation energy of the cations, calculated within the helium density functional theory approach, and their mutual Coulomb repulsion energy.

Time-resolved solvation of alkali ions in superfluid helium nanodroplets.

The sinking of alkali cations in superfluid 4He nanodroplets is investigated theoretically using liquid 4He time-dependent density functional theory at zero temperature. The simulations illustrate the dynamics of the buildup of the first solvation shell around the ions. The number of helium atoms in this shell is found to linearly increase with time during the first stages of the dynamics.

Observing the primary steps of ion solvation in helium droplets.

Solvation is a ubiquitous phenomenon in the natural sciences. At the macroscopic level, it is well understood through thermodynamics and chemical reaction kinetics. At the atomic level, the primary steps of solvation are the attraction and binding of individual molecules or atoms of a solvent to molecules or ions of a solute.

Quantized vortex nucleation in collisions of superfluid nanoscopic helium droplets at zero temperature.

We address the collision of two superfluid 4He droplets at non-zero initial relative velocities and impact parameters within the framework of liquid 4He time-dependent density functional theory at zero temperature. Despite the small size of these droplets (1000 He atoms in the merged droplet) imposed by computational limitations, we have found that quantized vortices may be readily nucleated for reasonable collision parameters. At variance with head-on collisions, where only vortex rings are produced, collisions with a non-zero impact parameter produce linear vortices that are nucleated at indentations appearing on the surface of the deformed merged droplet.

Superfluid helium droplet-mediated surface-deposition of neutral and charged silver atomic species.

Experimental and theoretical work has delivered evidence of the helium nanodroplet-mediated synthesis and soft-landing of metal nanoparticles, nanowires, clusters, and single atoms on solid supports. Recent experimental advances have allowed the formation of charged metal clusters into multiply charged helium nanodroplets. The impact of the charge of immersed metal species in helium nanodroplet-mediated surface deposition is proved by considering silver atoms and cations at zero-temperature graphene as the support.

Nanoscopic jets and filaments of superfluid He at zero temperature: A DFT study.

The instability of a cryogenic He jet exiting through a small nozzle into vacuum leads to the formation of He drops, which are considered ideal matrices for spectroscopic studies of embedded atoms and molecules. Here, we present a He-density functional theory (DFT) description of droplet formation resulting from jet breaking and contraction of superfluid He filaments. Whereas the fragmentation of long jets closely follows the predictions of linear theory for inviscid fluids, leading to droplet trains interspersed with smaller satellite droplets, the contraction of filaments with an aspect ratio larger than a threshold value leads to the nucleation of vortex rings, which hinder their breakup into droplets.

Diagnosis of Malnutrition According to GLIM Criteria Predicts Complications and 6-Month Survival in Cancer Outpatients.

Background and Aims: Malnutrition is a condition that has a great impact on oncology patients. Poor nutritional status is often associated with increased morbidity and mortality, increased toxicity, and reduced tolerance to chemotherapy, among other complications. The recently developed GLIM criteria for malnutrition aim to homogenize its diagnosis, considering the baseline disease status.

Clustering, collision, and relaxation dynamics in pure and doped helium nanoclusters: Density- vs particle-based approaches.

The clustering, collision, and relaxation dynamics of pristine and doped helium nanodroplets is theoretically investigated in cases of pickup and clustering of heliophilic argon, collision of heliophobic cesium atoms, and coalescence of two droplets brought into contact by their mutual long-range van der Waals interaction. Three approaches are used and compared with each other. The He time-dependent density functional theory method considers the droplet as a continuous medium and accounts for its superfluid character.

Dynamics of Photoexcited Cs Atoms Attached to Helium Nanodroplets.

We present an experimental study of the dynamics following the photoexcitation and subsequent photoionization of single Cs atoms on the surface of helium nanodroplets. The dynamics of excited Cs atom desorption and readsorption as well as CsHe exciplex formation are measured by using femtosecond pump-probe velocity map imaging spectroscopy and ion time-of-flight spectrometry. The time scales for the desorption of excited Cs atoms off helium nanodroplets as well as the time scales for CsHe exciplex formation are experimentally determined for the 6p states of Cs.

Unravelling the full relaxation dynamics of superexcited helium nanodroplets.

The relaxation dynamics of superexcited superfluid He nanodroplets is thoroughly investigated by means of extreme-ultraviolet (XUV) femtosecond electron and ion spectroscopy complemented by time-dependent density functional theory (TDDFT). Three main paths leading to the emission of electrons and ions are identified: droplet autoionization, pump-probe photoionization, and autoionization induced by re-excitation of droplets relaxing into levels below the droplet ionization threshold. The most abundant product ions are He2+, generated by droplet autoionization and by photoionization of droplet-bound excited He atoms.

Alkali atoms attached to vortex-hosting helium nanodroplets.

Light absorption or fluorescence excitation spectroscopy of alkali atoms attached to He droplets is investigated as a possible way for detecting the presence of vortices. To this end, we have calculated the equilibrium configuration and energetics of alkali atoms attached to a He droplet hosting a vortex line using He density functional theory. We use them to study how the dipole absorption spectrum of the alkali atom is modified when the impurity is attached to a vortex line.

Angular Momentum in Rotating Superfluid Droplets.

The angular momentum of rotating superfluid droplets originates from quantized vortices and capillary waves, the interplay between which remains to be uncovered. Here, the rotation of isolated submicrometer superfluid ^{4}He droplets is studied by ultrafast x-ray diffraction using a free electron laser. The diffraction patterns provide simultaneous access to the morphology of the droplets and the vortex arrays they host.

Rotating He droplets.

Motivated by recent experiments, we study normal-phase rotating He droplets within density functional theory in a semi-classical approach. The sequence of rotating droplet shapes as a function of angular momentum is found to agree with that of rotating classical droplets, evolving from axisymmetric oblate to triaxial prolate to two-lobed shapes as the angular momentum of the droplet increases. Our results, which are obtained for droplets of nanoscopic size, are rescaled to the mesoscopic size characterizing ongoing experimental measurements, allowing for a direct comparison of shapes.

Dynamics of impurity clustering in superfluid He nanodroplets.

The capture of multiple impurities by He droplets is investigated using real time dynamics within the density functional approach applied to liquid helium. We study the case of two or six Ar atoms colliding with a He droplet either in its ground state or hosting a six-vortex array. Depending on initial kinematic conditions, two different Ar structures are found: either a compact, gas-phase like cluster, or a loosely bound metastable cluster with helium density caged inside.

4s to 5s and 4p photoexcitation dynamics of K atoms from the surface of helium nanodroplets: a theoretical study.

We study the photodissociation of the potassium atom from a superfluid helium nanodroplet upon 5s 2S or 4p 2P excitation using the time-dependent helium density functional method (He-TDDFT). The importance of quantum effects is assessed by comparing the absorption spectrum obtained for a classical or a quantum description of the K atom. In the case of the 5s 2S ← 4s 2S excitation the difference is rather large, and we use a quantum description for the ensuing direct dissociation dynamics.

Impulsive alignment of He-CHI: A theoretical study.

We simulate the non-adiabatic laser alignment of the weakly bound He-CHI complex based on a quantum mechanical wave packet calculation for a model He-CHI interaction potential. Two different regimes are found depending on the laser intensity. At intensities typical of non-adiabatic alignment experiments, the rotational dynamics resembles that of the isolated molecule.

Helium-induced electronic transitions in photo-excited Ba-He exciplexes.

The possibility for helium-induced electronic transitions in a photo-excited atom is investigated using Ba excited to the 6p P state as a prototypical example. A diabatization scheme has been designed to obtain the necessary potential energy surfaces and couplings for complexes of Ba with an arbitrary number of helium atoms. It involves computing new He-Ba electronic wave functions and expanding them in determinants of the non-interacting complex.

Desorption dynamics of RbHe exciplexes off He nanodroplets induced by spin-relaxation.

Doped He nanodroplets are ideal model systems to study the dynamics of elementary photophysical processes in heterogeneous nanosystems. Here we present a combined experimental and theoretical investigation of the formation of free RbHe exciplex molecules from laser-excited Rb-doped He nanodroplets. Upon excitation of a droplet-bound Rb atom to the 5p3/22Π3/2-state, a stable RbHe exciplex forms within about 20 ps.

Capture of Xe and Ar atoms by quantized vortices in He nanodroplets.

We present a computational study, based on time-dependent Density Functional theory, of the real-time interaction and trapping of Ar and Xe atoms in superfluid He nanodroplets either pure or hosting quantized vortex lines. We investigate the phase-space trajectories of the impurities for different initial conditions and describe in detail the complex dynamics of the droplets during the capture of the impurities. We show that the interaction of the incoming atom with the vortex core induces large bending and twisting excitations of the vortex core lines, including the generation of helical Kelvin waves propagating along the vortex core.

Imaging Excited-State Dynamics of Doped He Nanodroplets in Real-Time.

The real-time dynamics of excited alkali metal atoms (Rb) attached to quantum fluid He nanodroplets is investigated using femtosecond imaging spectroscopy and time-dependent density functional theory. We disentangle the competing dynamics of desorption of excited Rb atoms off the He droplet surface and solvation inside the droplet interior as the Rb atom is ionized. For Rb excited to the 5p and 6p states, desorption occurs on starkly differing time scales (∼100 versus ∼1 ps, respectively).

Dynamics of photoexcited Ba(+) cations in (4)He nanodroplets.

We present a joint experimental and theoretical study on the desolvation of Ba(+) cations in (4)He nanodroplets excited via the 6p ← 6s transition. The experiments reveal an efficient desolvation process yielding mainly bare Ba(+) cations and Ba(+)Hen exciplexes with n = 1 and 2. The speed distributions of the ions are well described by Maxwell-Boltzmann distributions with temperatures ranging from 60 to 178 K depending on the excitation frequency and Ba(+) Hen exciplex size.

Communication: unraveling the (4)He droplet-mediated soft-landing from ab initio-assisted and time-resolved density functional simulations: Au@(4)He300/TiO2(110).

An ab-initio-based methodological scheme for He-surface interactions and zero-temperature time-dependent density functional theory for superfluid (4)He droplets motion are combined to follow the short-time collision dynamics of the Au@(4)He300 system with the TiO2(110) surface. This composite approach demonstrates the (4)He droplet-assisted sticking of the metal species to the surface at low landing energy (below 0.15 eV/atom), thus providing the first theoretical evidence of the experimentally observed (4)He droplet-mediated soft-landing deposition of metal nanoparticles on solid surfaces [Mozhayskiy et al.

Communication: A combined periodic density functional and incremental wave-function-based approach for the dispersion-accounting time-resolved dynamics of ⁴He nanodroplets on surfaces: ⁴He/graphene.

In this work we propose a general strategy to calculate accurate He-surface interaction potentials. It extends the dispersionless density functional approach recently developed by Pernal et al. [Phys.

Capture of heliophobic atoms by (4)He nanodroplets: the case of cesium.

Within Density Functional Theory (DFT), we address the capture of a Cs atom by a superfluid helium nanodroplet using models of different complexity. In the simplest model, the Cs-droplet potential is obtained in two extreme approximations, namely the sudden approximation in which one assumes that the density of the droplet is not relaxed as Cs approaches it, and the adiabatic approximation in which one assumes that it does. Next, a more complex approach in which the collision is described within a time-dependent DFT approach is employed.