Abstract Elastic, momentum-transfer (diffusion), and non-radiative charge-transfer cross sections are calculated for collisions between ground-state He + ( 2 S) ions and neutral He( 1 S) atoms over an energy range spanning fourteen orders of magnitude, from 10 −12 to 1 atomic unit. In this ultralow-energy regime, quantum mechanical effects dominate and the indistinguishability of helium nuclei necessitates a rigorous treatment of exchange symmetry. Phase shifts are computed using highly accurate ab initio potential energy curves for the X 2 Σ u and A 2 Σ g molecular states. The resulting elastic σ el , diffusion σ d , and charge-transfer σ ct cross sections reveal three distinct regimes: at energies below 10 −9 a.u., cross sections exceed 10 5 a 0 2 and are dominated by long-range polarization forces; in the intermediate range (10 −8 –10 −4 a.u.), pronounced quantum interference structures appear; at higher energies, results converge to semiclassical E −1/3 behavior. The data provide benchmark cross sections for ultracold ion–atom collision modeling relevant to cold-ion physics and hybrid atom–ion trapping experiments.
Previous semiempirical determinations by Fitzsimmons et al. of the asymptotic form of the potentials
Vg and
Vu for the helium molecular states $^{3}\ensuremath{\Sigma}_{g,u}^{+}$ are refined to include new experimental data. The resulting potentials yield cross sections for elastic scattering, diffusion, and metastability exchange in $\mathrm{He}(2^{3}S_{1})\ensuremath{-}\mathrm{H}\mathrm{e}(1^{1}S_{0})$ collisions in agreement with various experiments from 15 to 500 \ifmmode^\circ\else\textdegree\fi{}K.
Helium dimer in its metastable triplet electronic state, He
2(a 3Σu+), is a promising candidate for direct laser cooling and precision measurements. Interactions and collisions involving He
2(a 3Σu+) remain unexplored in ultracold and cold energy domains. Here, we present the first theoretical investigation of intermolecular interactions and collision dynamics of He
2(a 3Σu+)+Ne van der Waals complex. For the ground electronic state,
X 3A′, we employ a spin-restricted coupled cluster method with single, double, and noniterative triple excitations. The resulting interaction potential exhibits an extremely shallow well with a depth of 4.612 cm
−1. We construct a three-dimensional vibrationally averaged potential energy surface. Using this surface, we perform full close-coupling calculations including fine-structure levels of He
2(a 3Σu+) to investigate collisional excitation and quenching induced by Ne. We analyze the low-energy scattering dynamics and model resonant features associated with quasi-bound states supported by interaction potential. Propensity rule for fine-structure conserving transitions is established. We additionally consider He
2+Ar collisions and compare their energy dependence and resonance structure with those of He
2+Ne. The He
2+Ar system exhibits a richer resonance structure, highlighting the sensitivity of low-energy scattering to interaction potential and reduced mass. Calculated PES and scattering properties provide a reliable benchmark for description of He
2+Ne van der Waals complex and may be useful for interpretation of future experimental spectra and collision measurements.
The temperature dependence of conversion of $\rm He(2\sp3S\sb1)$ metastable atoms to $\rm He\sb2(a\sp3\Sigma\sbsp{u}{+})$ metastable molecules in the three-body reaction $\rm He(2\sp3S\sb1)+ 2He(1\sp1S\sb0)\to He\sb2(a\sp3\Sigma\sbsp{u}{+}) + He(1\sp1S\sb0)$ has been investigated over the temperature range 65K-700K. This reaction is thermally activated as a consequence of a long range repulsive barrier in the $\rm He(2\sp3S\sb1)-He(1\sp1S\sb0)$ interaction potential. The data reveal that there are two reaction channels with distinctly different activation energies. The temperature dependence of the measured rate coefficient k$\sb{\rm s}($T) is accurately described by $\rm k\sb{s}(T) = \lbrack 87.4\ T\ exp({-750}/T) + 4.1 T\ exp({-200}/T)\rbrack \times 10\sp{-37}\ cm\sp{-6}sec\sp{-1}$. The first activation energy, 750
± 70K (63
± 6meV), is equal to the known $\rm He(2\sp3S\sb1)$-$\rm He(1\sp1S\sb0)$ repulsive barrier height. The second activation energy is 17
± 2 meV. The temperature dependences of the rate constants for collision-induced mixing among $\rm He(2\sp3P\sb{J,m\sb{J}})$ levels, and for conversion of He(2$\sp3$P) atoms to $\rm He\sb2(b\sp3\Pi\sb{g})$ molecules in the three body reaction $\rm He(2\sp3P) + 2He(1\sp1S)\to He\sb2(b\sp3\Pi\sb{g}) + He(1\sp1S)$ have been investigated over the range 1.4$\sim$300K. The measured thermally-averaged cross section for $\rm He(2\sp3P\sb{J,m\sb{J}})$ mixing in collisions with ground state helium atoms are described by the function $\rm\sigma\sb{pm}(T) = (4.4 + 20.6/T\sp{1/3})\times 10\sp{-15}cm\sp2,$ and can be understood in terms of Langevin theory. The measured rate coefficients for the three body reaction exhibit a strong inverse temperature dependence, $\rm k\sb{p}(T) = (0.04 + 2.18/T)\times 10\sp{-30}\ cm\sp6{\cdot}s\sp{-1},$ which suggests that, unlike conversion of $\rm He(2\sp3S\sb1)$ to $\rm He\sb2(a\sp3\Sigma\sbsp{u}{+}),$ there is no activation energy required for this reaction. A magneto-optical trap for helium 2$\sp3$S metastable atoms has been designed and constructed, utilizing superconducting magnet gradient coils and a Ti:Sapphire ring laser for pumping the helium 2$\sp3$S-2$\sp3$P transition. He(2$\sp3$S) atoms are produced by a weak discharge in helium gas at temperature 1.3K. The discharge products flow through an orifice into the trap cell, where the He(2$\sp3$S) atoms are trapped and ground state helium atoms are rapidly cryopumped by zeolite pellets that cover most of the cell bottom. Preliminary experimental results suggest that $\sim
10\sp6$ atoms are trapped, with a trap lifetime of about 0.2 sec limited by He(2$\sp3$S) - He(2$\sp3$P) Penning reactions. Ultimately, it is estimated that a substantial number of atoms can be trapped and cooled for much longer times in a near-perfect vacuum. Measurements of decay times of the trapped atoms should yield rates for $\rm \sp{4,3}He(2\sp3S)$ - $\sp{4,3}$He(2$\sp3$S) and resonantly-enhanced He(2$\sp3$S) - He(2$\sp3$P) Penning reactions in the ultra-cold quantum regime, and perhaps the He(2$\sp3$S) natural lifetime.
In this thesis we investigate theoretically the cold collision properties of metastable neon (Ne*). The collisions of metastable rare gases (Rg*) exhibit a plethora of interesting phenomena: Due to the high internal excitation energies of the metastable atoms ionization processes are very likely. The produced ions can be detected with single-ion efficiency in the experiment. In experiments with atomic Rg* gases at cold temperatures T~1 mK, this allows for in-situ monitoring of the real-time dynamics of the atomic gas and for example for the study of two-particle correlations. Furthermore, in cold Rg* gases one can examine the prospects of creating a Bose-Einstein condensate or a degenerate Fermi gas of Rg*. Ne* is a promising candidate for Bose-Einstein condensation and in the group of G. Birkl the properties of cold gases of Ne* are investigated experimentally. Two-body loss rate coefficients due to the ionization processes and elastic cross sections have been measured. It is useful to complement the experimental measurements with a theoretical study in order to obtain a better understanding of the cold Ne* gases and the collision physics of Ne*. At the low temperatures of the atomic gases, these gases are dilute with particle number densities of n~10^9 cm^{-3}. For these low densities, the behavior of the gas is determined mainly by two-body collision physics which is solved by quantum scattering theory in terms of the S matrix. The collision physics is given by short-range interactions and long-range interactions of the atoms. The short-range and long-range interaction potentials of Ne* have been calculated in the molecular basis of Ne2. In this thesis we first calculate short-range and long-range interactions of atoms and molecular basis states of diatomic molecules with a simpler electronic structure than Ne* and Ne2 in order to introduce the notation and to discuss the characteristics of the calculated molecular interaction potentials and in order to employ them in the scattering calculations for Ne*. Instead of solving the full scattering equations by taking into account all the molecular interaction potentials, we demonstrate that the collision physics of Ne* can be described in terms of a coupled two-channel model with a single interaction potential only which describes the elastic scattering of Ne*. In this model, ionization in Ne* collisions is described by the transition of the upper elastic interaction channel to the lower channel, representing the loss or ionization channel. We introduce two versions of the two-channel model in this work. In the first version, the two channels are given by square-well potentials. We can solve the scattering equations analytically and for complex wave numbers k and study the solutions in the complex k plane. With an expansion of the S matrix in terms of its poles in the complex k plane we find a parametrization of the two-body loss rate coefficients. We show that these coefficients describe ionizing collisions of Ne* by comparing them to the experimental measurements and to the numerical results obtained by the two-channel model in the second version. In this second version of the two-channel model, the elastic scattering channel is given by a realistic interaction potential of Ne*, consisting of a calculated short-range and long-range molecular potential, and the loss channel by a model ionization potential. For this model we calculate the two-body loss rate coefficients and the elastic cross sections for the isotope mixtures of Ne* which have been measured experimentally and demonstrate that the free potential parameters can be optimized to the experimental data to achieve very good agreement of the numerical results with the experimental measurements. We discuss the validity of the two-channel model by comparing the results to existing models for cold Rg* collisions and find that the two-channel model of this work is a useful extension to these models.