Time-resolved solvation dynamics of Li$^+$, Na$^+$ and K$^+$ ions in liquid helium nanodroplets

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Main Authors: Christensen, Jeppe K., Albrechtsen, Simon H., Petersen, Christian E., Schouder, Constant A., Sánchez-Pérez, Iker, Carchi-Villalta, Pedro Javier, Bartolomei, Massimiliano, Pirani, Fernando, González-Lezana, Tomás, Stapelfeldt, Henrik
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Published: 2025
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author Christensen, Jeppe K.
Albrechtsen, Simon H.
Petersen, Christian E.
Schouder, Constant A.
Sánchez-Pérez, Iker
Carchi-Villalta, Pedro Javier
Bartolomei, Massimiliano
Pirani, Fernando
González-Lezana, Tomás
Stapelfeldt, Henrik
author_facet Christensen, Jeppe K.
Albrechtsen, Simon H.
Petersen, Christian E.
Schouder, Constant A.
Sánchez-Pérez, Iker
Carchi-Villalta, Pedro Javier
Bartolomei, Massimiliano
Pirani, Fernando
González-Lezana, Tomás
Stapelfeldt, Henrik
contents In 2023, ultrafast pump-probe spectrocopy was used to record the solvation dynamics of a single Na$^+$ ion in a liquid helium droplet, atom-by-atom and with femtosecond time resolution [Albrechtsen \textit{et al., Nature}, 2023, \textbf{623}, 319]. Subsequently, theoretical studies showed that other alkali ions solvate in a similar manner but no experimental results were reported so far. Here, we extend the previous measurement on Na$^+$ to Li$^+$ and K$^+$ ions. A pump pulse selectively ionizes an alkali atom, initially residing at the droplet surface, and the ensuing solvation dynamics of the formed alkali cation, Ak$^+$, is followed by ionizing a Xe atom, located in the droplet interior, and recording the yields of Ak$^+$He$_n$ ions expelled from the droplet as a function of the pump-probe pulse delay. We find that Li$^+$, Na$^+$ and K$^+$ ions solvate with a binding rate of 1.8 $\pm$ 0.1, 1.8 $\pm$ 0.1 and 1.7 $\pm$ 0.1 He per ps, respectively. Furthermore, by comparing the number distribution of the Ak$^+$He$_n$ ion yields to the evaporation energies of these ion--He complexes, obtained by Path Integral Monte Carlo calculations, we identify signatures of the first solvation shells of Li$^+$, Na$^+$ and K$^+$. Lastly, we determine the time-dependent dissipation of the solvation energy from the vicinity of the three alkali ion species and find that the rate is highest (lowest) for Li$^+$ (K$^+$)
format Preprint
id arxiv_https___arxiv_org_abs_2510_12330
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Time-resolved solvation dynamics of Li$^+$, Na$^+$ and K$^+$ ions in liquid helium nanodroplets
Christensen, Jeppe K.
Albrechtsen, Simon H.
Petersen, Christian E.
Schouder, Constant A.
Sánchez-Pérez, Iker
Carchi-Villalta, Pedro Javier
Bartolomei, Massimiliano
Pirani, Fernando
González-Lezana, Tomás
Stapelfeldt, Henrik
Chemical Physics
In 2023, ultrafast pump-probe spectrocopy was used to record the solvation dynamics of a single Na$^+$ ion in a liquid helium droplet, atom-by-atom and with femtosecond time resolution [Albrechtsen \textit{et al., Nature}, 2023, \textbf{623}, 319]. Subsequently, theoretical studies showed that other alkali ions solvate in a similar manner but no experimental results were reported so far. Here, we extend the previous measurement on Na$^+$ to Li$^+$ and K$^+$ ions. A pump pulse selectively ionizes an alkali atom, initially residing at the droplet surface, and the ensuing solvation dynamics of the formed alkali cation, Ak$^+$, is followed by ionizing a Xe atom, located in the droplet interior, and recording the yields of Ak$^+$He$_n$ ions expelled from the droplet as a function of the pump-probe pulse delay. We find that Li$^+$, Na$^+$ and K$^+$ ions solvate with a binding rate of 1.8 $\pm$ 0.1, 1.8 $\pm$ 0.1 and 1.7 $\pm$ 0.1 He per ps, respectively. Furthermore, by comparing the number distribution of the Ak$^+$He$_n$ ion yields to the evaporation energies of these ion--He complexes, obtained by Path Integral Monte Carlo calculations, we identify signatures of the first solvation shells of Li$^+$, Na$^+$ and K$^+$. Lastly, we determine the time-dependent dissipation of the solvation energy from the vicinity of the three alkali ion species and find that the rate is highest (lowest) for Li$^+$ (K$^+$)
title Time-resolved solvation dynamics of Li$^+$, Na$^+$ and K$^+$ ions in liquid helium nanodroplets
topic Chemical Physics
url https://arxiv.org/abs/2510.12330