The dynamics of Na atoms on the surface of helium nanodroplets following excitation via the 3p ← 3s transition has been investigated using state-specific ion-based detection of the products. Excitation of the system to the 3p (2)Π states is found to lead to the desorption of both bare Na and NaHe exciplexes. The associated speed distributions point to an impulsive desorption process for Na products and a thermally driven process for the NaHe exciplexes. In contrast, excitation of the 3p (2)Σ state leads exclusively to the impulsive desorption of Na atoms. In this case, the desorption is accompanied by a helium-induced relaxation process, as evidenced by the large fraction of detected Na (2)P1/2 atoms. The relaxation process is thought to be related to a crossing between the (2)Π1/2 and (2)Σ potential energy curves at large distance.
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J Chem Phys
December 2024
Departament FQA, Facultat de Física, Universitat de Barcelona, Av. Diagonal 645, 08028 Barcelona, Spain.
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.
View Article and Find Full Text PDFJ Chem Phys
December 2024
Department of Chemistry, Aarhus University, Langelandsgade 140, 8000 Aarhus C, Denmark.
Vibrational wave packets are created in the lowest triplet state 13Σu+ of K2 and Rb2 residing on the surface of helium nanodroplets, through non-resonant stimulated impulsive Raman scattering induced by a moderately intense near-infrared laser pulse. A delayed, intense 50-fs laser pulse doubly ionizes the alkali dimers via multiphoton absorption and thereby causes them to Coulomb explode into a pair of alkali ions Ak+. From the kinetic energy distribution P(Ekin) of the Ak+ fragment ions, measured at a large number of delays, we determine the time-dependent internuclear distribution P(R, t), which represents the modulus square of the wave packet within the accuracy of the experiment.
View Article and Find Full Text PDFJ Phys Chem A
December 2024
Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States.
J Chem Phys
November 2024
Université Paris-Saclay, Univ Evry, CY Cergy Paris Université, CNRS, LAMBE, Evry-Courcouronnes 91025, France.
The collision of cesium atoms on the surface of helium nanodroplets (HNDs) containing 1000 atoms is described by the ZPAD-mPL approach, a zero-point averaged dynamics (ZPAD) method based on a He-He pseudopotential adjusted to better reproduce the total energy of He1000. Four types of collisional patterns were identified depending on the initial projectile speed v0 and impact parameter b. At the lowest speeds (v0 ≲ 250 m s-1), Cs atoms are softly captured by the HND surface, while at the highest ones (v0 ≳ 500-600 m s-1), Cs atoms can travel through the droplet and move away.
View Article and Find Full Text PDFRep Prog Phys
November 2024
Department of Physics and Astronomy, Aarhus University, 8000 Aarhus, C, Denmark.
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