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arXiv:2012.15536 · Physical Review A

Rydberg atom-ion collisions in cold environments

Henrik Hirzler, Jesús Pérez‐Ríos

Published Apr 19, 2021• 12 citations
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Abstract

Low-energy collisions of Rydberg atom-ion systems are investigated theoretically. We present the parameter space associated with suitable approaches for the dynamics of Rydberg atom-ion collisions, i.e., quantum, Langevin, and classical exchange regimes, showing that for the lowest reachable temperatures a classical treatment is appropriate. A quasiclassical trajectory method is used to study charge exchange cross sections for ${\mathrm{Li}}^{*}\text{\ensuremath{-}}{\mathrm{Li}}^{+}$ and ${\mathrm{Li}}^{*}\text{\ensuremath{-}}{\mathrm{Cs}}^{+}$ at collision energies down to $1\phantom{\rule{0.28em}{0ex}}\mathrm{K}$. For cold collisions we find the charge exchange cross section deviating from the ${n}^{4}$ geometric scaling. Furthermore, for low-energy collisions, we find both an influence of the ionic core repulsion as well as variations for two different models used for describing the electron-core potential.

DOI
10.1103/physreva.103.043323

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•Jan 1, 2003•1 citation
Low-energy collisions of Rydberg atom-ion systems are investigated theoretically. We present the parameter space associated with suitable approaches for the dynamics of Rydberg atom-ion collisions, i.e., quantum, Langevin, and classical exchange regimes, showing that for the lowest reachable temperatures a classical treatment is appropriate. A quasiclassical trajectory method is used to study charge exchange cross sections for Li∗\ensuremath-Li+{\mathrm{Li}}^{*}\text{\ensuremath{-}}{\mathrm{Li}}^{+}Li∗\ensuremath-Li+ and Li∗\ensuremath-Cs+{\mathrm{Li}}^{*}\text{\ensuremath{-}}{\mathrm{Cs}}^{+}Li∗\ensuremath-Cs+ at collision energies down to 1K1\phantom{\rule{0.28em}{0ex}}\mathrm{K}1K. For cold collisions we find the charge exchange cross section deviating from the n4{n}^{4}n4 geometric scaling. Furthermore, for low-energy collisions, we find both an influence of the ionic core repulsion as well as variations for two different models used for describing the electron-core potential.
Charge transfer collisions between slow ions and Rydberg atoms have been studied for ion charges q=1−−4q\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}1--4q=1−−4, using resonant laser excitation to detect specific energy states of the collision products. The data collected show a clear resonance in the capture cross section to a particular energy state as the binding energy of the Rydberg target is varied. The resonance position differs significantly from the predictions of the classical overbarrier model, and its width becomes very small (0.025 eV) at the lowest velocities studied.
We report on the observation of cold collisions between 6Li^{6}\mathrm{Li}6Li atoms and Yb+{\mathrm{Yb}}^{+}Yb+ ions. This combination of species has recently been proposed as the most suitable for reaching the quantum limit in hybrid atom-ion systems, due to its large mass ratio. For atoms and ions prepared in the 2S1/2^{2}S_{1/2}2S1/2​ ground state, the charge-transfer and association rate is found to be at least 103{10}^{3}103 times smaller than the Langevin collision rate. These results confirm the excellent prospects of $^{6}\mathrm{Li}\ensuremath{-}{\mathrm{Yb}}^{+}$ for sympathetic cooling and quantum information applications. For ions prepared in the excited electronic states 2P1/2,2D3/2^{2}P_{1/2}, ^{2}D_{3/2}2P1/2​,2D3/2​, and 2F7/2^{2}F_{7/2}2F7/2​, we find that the reaction rate is dominated by charge transfer and does not depend on the ionic isotope or the collision energy in the range $\ensuremath{\sim}1--120\phantom{\rule{0.16em}{0ex}}\mathrm{mK}$. The low charge-transfer rate for ground-state collisions is corroborated by theory, but the 4f4f4f shell in the Yb+{\mathrm{Yb}}^{+}Yb+ ion prevents an accurate prediction for the charge-transfer rate of the 2P1/2,2D3/2^{2}P_{1/2}, ^{2}D_{3/2}2P1/2​,2D3/2​, and 2F7/2^{2}F_{7/2}2F7/2​ states. Using ab initio methods of quantum chemistry we calculate the atom-ion interaction potentials up to energies of $30\ifmmode\times\else\texttimes\fi{}{10}^{3}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$, and use these to give qualitative explanations of the observed rates.
Atoms in highly excited Rydberg states possess physical characteristics quite unlike those associated with atoms in the ground or low-lying excited states. In particular, they are physically very large and are only very weakly bound. In consequence, collisions can lead to a wide variety of reaction processes many of which are unique to Rydberg species and have very large collision cross sections. In collisions with neutral targets, Rydberg atoms behave not as an atom but rather as a pair of well-separated independent scatterers, namely the core ion and the excited Rydberg electron. In the present article we discuss many of the different reactions that can occur when Rydberg atoms collide with neutral targets, focusing principally on reactions that are dominated by (binary) Rydberg electron-target interactions and include collisions with molecules that attach free low-energy electrons and with polar targets. In certain situations, however, interactions involving the Rydberg core ion are important. This is illustrated using as an example the destruction of ultralong-range Rydberg molecules excited in a cold dense gas.
Charge-transfer collisions between slow multiply charged ions and highly excited Rydberg atoms have been studied to determine the details of the internal energy transfer accompanying charge exchange. The experiment uses lasers to define uniquely the binding energies of both initial and final states of the collision, thereby eliminating the ambiguity inherent in the selective field ionization method used for previous studies. The results clearly characterize the capture energetics over the range of ion charge q=1−−11q=1--11q=1−−11 and velocity v=0.031−−0.138a.u.v=0.031--0.138\mathrm{a}.\mathrm{u}.v=0.031−−0.138a.u. The measurements are in very good agreement with predictions of the classical trajectory Monte Carlo method, but not with predictions of other classical models.
The aim of this work is to investigate the dynamics of collisions between ions and Rydberg atoms by using the Classical Trajectory Monte Carlo (CTMC) method. The study is started by collisions with oriented elliptical Rydberg atom, is then continued to collisions involving hydrogen Rydberg target in an external magnetic field in the l-mixing regime, and later arrives at antihydrogen formation in an external magnetic field where Rydberg positronium is taken as target.\nThe CTMC method has been applied in the study. For different targets, the CTMC method had to be adjusted and reconstructed to properly create the initial target state for the quasi-separable one-body initial system (hydrogen target) and the two-body initial system (positronium target). Charge exchange and ionization cross sections are calculated under special consideration of different initial target states.\nThe velocity matching phenomenon and Thomas capture which appears in the upstream-downstream asymmetry are found in ion-oriented elliptical Rydberg atom collisions, reflecting the important roles of the initial electron spatial and momentum distributions. By increasing the projectile charge, the distortion of the initial states caused by the strong perturbation of approaching projectile induces pronounced changes in the momentum distribution.\nIn the collisions involving hydrogen Rydberg atoms in a magnetic field, a cross section reduction in case of an increasing magnetic field is found for multiply charged projectiles. The structure effect due to the influence of the magnetic field on the initial state distribution results in different capture cross sections for two characterized, kmax and kmin, states. The velocity matching phenomenon as well as the effect of multiply charged projectile ion are observed in the collisions.\nFurthermore, antihydrogen formation in a magnetic field has been studied. Rydberg positroniums are assumed to be the target atoms, colliding with antiprotons. The initial target positronium state is carefully constructed by means of a newly introduced conserved operator, the pseudomomentum K. Similar properties as in the previous hydrogen target atom case were investigated. It is found that the existence of the magnetic field changes the spatial distribution of positronium to irregular motion. By increasing the magnetic field, it induces a decrease of the resulting capture cross sections (i.e. the antihydrogen formation). Thomas capture which happens in the collision plane in the field-free case is foiled. A smaller positronium binding energy and a larger geometrical extension of the target positronium atom yield a larger capture cross section.