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.
View Article and Find Full Text PDFThe 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.
View Article and Find Full Text PDFWe 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.
View Article and Find Full Text PDFDoped 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.
View Article and Find Full Text PDFPhys Chem Chem Phys
September 2017
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.
View Article and Find Full Text PDFThe 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).
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