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Physical Review A

Energy distributions of He+ and He2+ ions formed in ultracold He(23S1)+He(23P2) collisions

Marc Pieksma, Martin Čížek, Jan W. Thomsen, P. van der Straten, Arend Niehaus

Published Aug 9, 2002• 5 citations
Publisher

Abstract

Energy distributions of ${\mathrm{He}}^{+}$ and ${\mathrm{He}}_{2}^{+}$ ions produced in ultracold $\mathrm{He}(2{}^{3}{S}_{1})+\mathrm{He}(2{}^{3}{P}_{2})$ collisions are presented. These helium metastable atoms are trapped and cooled in a magneto-optical trap, and have a temperature of $1.1\ifmmode\pm\else\textpm\fi{}0.2 \mathrm{mK}.$ Initial kinetic energies of the product ${\mathrm{He}}^{+}$ and ${\mathrm{He}}_{2}^{+}$ ions are analyzed in energy, using a weak electrostatic extraction field in combination with a time-of-flight technique. A pronounced structure is observed in the ${\mathrm{He}}^{+}$ ion distribution, which can be well explained by a theoretical model that considers the avoided crossings between only three metastable ${}^{3}{\ensuremath{\Sigma}}_{\mathrm{g}}^{+}$ states of the transient ${\mathrm{He}}_{2}$ molecule. The measured ${\mathrm{He}}_{2}^{+}$ distribution has a width that is consistent with the maximum recoil energy of 1.1 meV.

DOI
10.1103/physreva.66.022703

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Energy distributions of He+{\mathrm{He}}^{+}He+ and He2+{\mathrm{He}}_{2}^{+}He2+​ ions produced in ultracold He(23S1)+He(23P2)\mathrm{He}(2{}^{3}{S}_{1})+\mathrm{He}(2{}^{3}{P}_{2})He(23S1​)+He(23P2​) collisions are presented. These helium metastable atoms are trapped and cooled in a magneto-optical trap, and have a temperature of 1.1\ifmmode±\else\textpm\fi0.2mK.1.1\ifmmode\pm\else\textpm\fi{}0.2 \mathrm{mK}.1.1\ifmmode±\else\textpm\fi0.2mK. Initial kinetic energies of the product He+{\mathrm{He}}^{+}He+ and He2+{\mathrm{He}}_{2}^{+}He2+​ ions are analyzed in energy, using a weak electrostatic extraction field in combination with a time-of-flight technique. A pronounced structure is observed in the He+{\mathrm{He}}^{+}He+ ion distribution, which can be well explained by a theoretical model that considers the avoided crossings between only three metastable 3\ensuremathΣg+{}^{3}{\ensuremath{\Sigma}}_{\mathrm{g}}^{+}3\ensuremathΣg+​ states of the transient He2{\mathrm{He}}_{2}He2​ molecule. The measured He2+{\mathrm{He}}_{2}^{+}He2+​ distribution has a width that is consistent with the maximum recoil energy of 1.1 meV.
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 ±\pm± 70K (63 ±\pm± 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 ±\pm± 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 $\sim101010\sp6$ 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.
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We report the measurement of collision rate coefficient for collisions between ultracold Cs atoms and low-energy Cs+\mathrm{C}{\mathrm{s}}^{+}Cs+ ions. The experiments are performed in a hybrid trap consisting of a magneto-optical trap (MOT) for Cs atoms and a Paul trap for Cs+\mathrm{C}{\mathrm{s}}^{+}Cs+ ions. The ion-atom collisions impart kinetic energy to the ultracold Cs atoms, resulting in their escape from the shallow MOT and, therefore, in a reduction in the number of Cs atoms in the MOT. By monitoring, using fluorescence measurements, the Cs atom number, and the MOT loading dynamics and then fitting the data to a rate equation model, the ion-atom collision rate is derived. The $\mathrm{Cs}\ensuremath{-}\mathrm{C}{\mathrm{s}}^{+}$ collision rate coefficient $9.3(\ifmmode\pm\else\textpm\fi{}0.4)(\ifmmode\pm\else\textpm\fi{}1.2)(\ifmmode\pm\else\textpm\fi{}3.5)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}\phantom{\rule{0.16em}{0ex}}{\mathrm{m}}^{3}\phantom{\rule{0.28em}{0ex}}{\mathrm{s}}^{\ensuremath{-}1}$, measured for an ion distribution with most probable collision energy of 95 meV $(\ensuremath{\approx}{\mathrm{k}}_{\mathrm{B}}\phantom{\rule{4pt}{0ex}}1100\phantom{\rule{4pt}{0ex}}\mathrm{K})$, is in fair agreement with theoretical calculations. As an intermediate step, we also determine the photoionization cross section of Cs 6P3/26{P}_{3/2}6P3/2​ atoms at 473 nm wavelength to be $2.28(\ifmmode\pm\else\textpm\fi{}0.33)\phantom{\rule{4pt}{0ex}}\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}21}\phantom{\rule{0.16em}{0ex}}{\mathrm{m}}^{2}$.
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We have studied the dynamic properties of the He(23S)\mathrm{He}(2^{3}S)He(23S) and the ${\mathrm{He}}_{2}(a^{3}\ensuremath{\Sigma}_{u}^{+})$ atomic and molecular metastable states of helium that are produced in electron-bombarded superfluid helium. The steady-state concentration of ${\mathrm{He}}_{2}(a^{3}\ensuremath{\Sigma}_{u}^{+})$ molecules is shown to be limited by collisions between pairs of these molecules. Measurements of the rate coefficient for this bimolecular reaction as a function of temperature and pressure show that the reaction is diffusion limited and that the diffusion coefficient for the metastable molecules in the superfluid is determined by ${\mathrm{He}}_{2}(a^{3}\ensuremath{\Sigma}_{u}^{+})$-roton collisions. The bilinear destruction of metastable molecules has been monitored for times as long as 0.1 sec after the initial population of the state, and this establishes a lower bound of 0.1 sec on the radiative lifetime of the $(v=0) {\mathrm{He}}_{2}(a^{3}\ensuremath{\Sigma}_{u}^{+})$ state in superfluid helium. The lifetime and decay mode of the He(23S)\mathrm{He}(2^{3}S)He(23S) atoms are distinctly different from that of the corresponding ${\mathrm{He}}_{2}(a^{3}\ensuremath{\Sigma}_{u}^{+})$ molecule. In particular, the characteristic lifetime of the He(23S)\mathrm{He}(2^{3}S)He(23S) state in superfluid helium is essentially independent of the temperature between 2.08 and 1.4 \ifmmode^\circ\else\textdegree\fi{}K and is measured to be about 15 \ensuremath{\mu}sec. Our experimental observations indicate that the destruction of metastable atoms results in the population of high vibrational levels of the $a^{3}\ensuremath{\Sigma}_{u}^{+}$ molecular state. However, it is shown that the production of $(v=0) {\mathrm{He}}_{2}(a^{3}\ensuremath{\Sigma}_{u}^{+})$ molecules responds immediately to the electron beam (response time 3 \ensuremath{\mu}sec) and thus the formation of this state in the liquid does not depend upon the destruction of metastable atoms. Despite the fact that the lifetimes and decay modes of the metastable He(23S)\mathrm{He}(2^{3}S)He(23S) atoms and $(v=0) {\mathrm{He}}_{2}(a^{3}\ensuremath{\Sigma}_{u}^{+})$ molecules are not related, the production rates for these states are nearly equal and correspond to about 450 and 500 per incident 160-keV electron, respectively.
Superfluid helium nanodroplets are used to cool ions and form ion-neutral clusters at a temperature of 0.37 K. A desolvation technique was developed that allowed for the study of captured ions by mass spectrometry. From the mass spectrometry results it was determined that helium droplets may successfully capture sodium cations with kinetic energy of ~200 eV. Clusters of the neutral molecules H2O, N2, and HCN with Na+ were observed. Based on binding strength considerations, it is argued that the desolvation process imparts little energy into the ion-neutral clusters, avoiding dissociation. This result leads to the conclusion that ion-neutral clusters are formed within the droplet prior to desolvation, indicating that the helium snowball that is assumed to form around Na+ does not prevent ion-neutral cluster formation. This conclusion is supported by ab initio calculations, the results of which indicate the presence of barrierless pathways for neutral molecule insertion into the helium snowball surrounding Na+. The process of ion capture by helium droplets was studied by comparison of measured ion-doped droplet size distributions to known pre-ion capture droplet size distributions. The measured ion-doped droplet size distributions were affected by nozzle temperature, ion kinetic energy, and ion mass. These factors primarily affect two parameters of the ion-doped droplet size distribution, the minimum droplet size threshold, Nthr, and the droplet size at maximum signal intensity, Nmax. The effects of the studied factors on the measured distributions cannot be explained in terms of currently accepted droplet cooling mechanisms. Analysis of the results suggests that droplet doping efficiency can be improved in several ways, including a higher flux of lower-energy ions. An apparatus for the production and focusing of alkali cations at high fluxes and low energies is described. This apparatus was able to produce higher ion currents at lower kinetic energies than previous ion sources.