Charge Exchange Dynamics in Cold Collisions of $^{40}$CaH$^+$ and $^{39}$K
Lawrence Berkeley National Lab（劳伦斯伯克利国家实验室）；Duke Quantum Center, Duke University（杜克大学量子中心）；Department of Physics, Duke University（杜克大学物理系）；Faculty of Physics, University of Warsaw（华沙大学物理学院）；IonQ Inc（IonQ公司）；Department of Electrical and Computer Engineering, Duke University（杜克大学电气与计算机工程系）；Department of Chemistry, Duke University（杜克大学化学系）
Swapnil Patel, Dibyendu Sardar, Jyothi Saraladevi, Michał Tomza, Kenneth R. Brown
We report the observation of charge-exchange collisions between trapped calcium monohydride molecular ions ($^{40}$CaH$^+$) and ultracold potassium atoms ($^{39}$K) in a hybrid ion-atom trap. The measured charge-exchange rate coefficient is significantly suppressed relative to the Langevin rate constant for the system. We use $\mathit{ab\ initio}$ quantum-chemical calculations to model the (CaH-K)$^+$ complex in the ground and excited electronic states and to identify possible charge-exchange mechanisms. Our calculations rule out a direct non-radiative charge-exchange reaction and instead point to a radiative mechanism, but do not quantitatively reproduce the measured rate, highlighting the need for a full-dimensional quantum dynamics treatment that includes vibrational motion and intermediate complex formation. Our work demonstrates that cold hybrid ion-atom platforms with molecular ions enable access to richer chemical complexity and collisional dynamics inaccessible in purely atomic systems.
We use quantum and classical adiabatic capture theories to study the chemical reaction Li + CaH -> LiH + Ca. Using a recently developed ab initio potential energy surface, which provides an accurate representation of long-range interactions in the entrance reaction channel, we calculate the adiabatic channel potentials by diagonalizing the atom-molecule Hamiltonian as a function of the atom-molecule separation. The resulting adiabatic channel potentials are used to calculate both the classical and quantum capture probabilities as a function of collision energy, as well as the temperature depen…
We report the sympathetic cooling and Coulomb crystallization of molecular ions above the surface of an ion-trap chip. N$_2^+$ and CaH$^+$ ions were confined in a surface-electrode radiofrequency ion trap and cooled by the interaction with laser-cooled Ca$^{+}$ ions to secular translational temperatures in the millikelvin range. The configuration of trapping potentials generated by the surface electrodes enabled the formation of planar bicomponent Coulomb crystals and the spatial separation of the molecular from the atomic ions on the chip. The structural and thermal properties of the Coulomb …
We present a combined experimental and theoretical study of cold reactive collisions between laser-cooled Ca+ ions and Rb atoms in an ion-atom hybrid trap. We observe rich chemical dynamics which are interpreted in terms of non-adiabatic and radiative charge exchange as well as radiative molecule formation using high-level electronic structure calculations. We study the role of light-assisted processes and show that the efficiency of the dominant chemical pathways is considerably enhanced in excited reaction channels. Our results illustrate the importance of radiative and non-radiative process…
We report a study of cold charge-transfer (CT) collisions of Rb atoms with N$_2^+$ and O$_2^+$ ions in the mK regime using a dynamic ion-neutral hybrid trapping experiment. State- and collision-energy- dependent reaction rate coefficients have been measured for both systems. We observe markedly different charge-transfer kinetics and dynamics for the different systems and reaction channels. While the kinetics in some channels are consistent with classical capture theory for the rate coefficient, others show distinct non-universal dynamics. The experimental results are interpreted with the help …
We present a method for generating cold neutral atoms via charge exchange reactions between trapped ions and Rydberg positronium. The high charge exchange reaction cross section leads to efficient neutralisation of the ions and since the positronium-ion mass ratio is small, the neutrals do not gain appreciable kinetic energy in the process. When the original ions are cold the reaction produces neutrals that can be trapped or further manipulated with electromagnetic fields. Because a wide range of species can be targeted we envisage that our scheme may enable experiments at low temperature that…
Employing a two-stage cryogenic buffer gas cell, we produce a cold, hydrodynamically extracted beam of calcium monohydride molecules with a near effusive velocity distribution. Beam dynamics, thermalization and slowing are studied using laser spectroscopy. The key to this hybrid, effusive-like beam source is a "slowing cell" placed immediately after a hydrodynamic, cryogenic source [Patterson et al., J. Chem. Phys., 2007, 126, 154307]. The resulting CaH beams are created in two regimes. One modestly boosted beam has a forward velocity of vf = 65 m/s, a narrow velocity spread, and a flux of 10^…
The relevance of magnetic impurity problems in cold atom systems depends crucially on the nature of exchange interaction between itinerant fermionic atoms and a localized impurity atom. In particular, Kondo physics occurs only if the exchange interaction is anti-ferromagnetic, and strong enough to yield high enough Kondo temperature ($T_K/T_F \ge 0.1$). Focusing, as an example, on the experimentally accessible system of ultra-cold $^{173}$Yb atoms, it is shown that the sign and strength of an exchange interaction between an itinerant Yb($^{1}$S$_{0}$) atom and a trapped Yb($^{3}$P$_{0}$) atom …
The s-wave elastic phase-shifts and s-wave elastic cross sections are studied to find the effect of long-range forces on cold-atomic interactions using a modified static-exchange model for Ps-H system. A Feshbach resonance in the triplet channel using the modified static-exchange model at the energy ~ 3x10^{-6} eV caused by long-range forces in the Ps-H system is being reported.
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 quasi-classical trajectory method is used to study charge exchange cross sections for Li$^*$-Li$^+$ and Li$^*$-Cs$^+$ at collision energies down to $1\,$K. For cold collisions we find the charge exchange cross section deviating from the $n^4$ geometric sc…
We show that the integral cross sections for state-to-state quantum scattering of cold molecules in a magnetic field can be efficiently computed using the total angular momentum representation despite the presence of unphysical Zeeman states in the eigenspectrum of the asymptotic Hamiltonian. We demonstrate that the unphysical states arise due to the incompleteness of the space-fixed total angular momentum basis caused by using a fixed cutoff value $J_\text{max}$ for the total angular momentum of the collision complex $J$. As a result, certain orbital angular momentum ($l$) basis states lack t…
We demonstrate a dual-axis accelerometer and gyroscope atom interferometer, which forms the building blocks of a six-axis inertial measurement unit. By recapturing the atoms after the interferometer sequence, we maintain a large atom number at high data-rates of 50 to 100 measurements per second. Two cold ensembles are formed in trap zones located a few centimeters apart, and are launched toward one-another. During their ballistic trajectory, they are interrogated with a stimulated Raman sequence, detected, and recaptured in the opposing trap zone. We achieve sensitivities at $\mathrm{μ\mathit…
Exchange in a Boltzmann gas of bosons with several internal states leads to collective transport of internal polarization. The internal dynamics can be understood as Larmor precession in the presence of a torque induced by atoms on each other via exchange coupling. A generalized Bloch equation that includes interatomic exchange effects as well as orbital motion in the gas is derived and used to interpret recent experiment by Lewandowski et al. as an excitation of a collective wave of internal state polarization. It is shown that exchange leads to formation of domains in which precession freque…
The static-exchange model (SEM) and the modified static-exchange model (MSEM) recently introduced by Ray [1] is applied to study the elastic collision between two hydrogen-like atoms when both are in ground states considering the system as a four-body Coulomb problem in the center of mass frame, in which all the Coulomb interaction terms in direct and exchange channels are treated exactly. The SEM includes the non-adiabatic short-range effect due to electron-exchange. The MSEM added in it, the long-range effect due to induced dynamic dipole polarizabilities between the atoms e.g. the Van der W…
The antihydrogen formation by charge exchange between cold antiprotons and Rydberg positronium Ps is studied by using the Classical Trajectory Monte Carlo (CTMC) method.
We discuss theoretically the optical binding of one-dimensional chains of cold atoms shone by a transverse pump, where particles self-organize to a distance close to an optical wavelength. As the number of particles is increased, the trapping potential increases logarithmically as the contributions from all atoms add up constructively. We identify a cooperative cooling mechanism, due to the mutual exchange of photons between atoms, which can beat the spontaneous emission for chains that are long enough. Surprisingly, the cooling is optimal very close to the resonance. This peculiar cooling mec…
We demonstrate a double-trap system well suited to study cold collisions between trapped ions and trapped atoms. Using Yb$^+$ ions confined in a Paul trap and Yb atoms in a magneto-optical trap, we investigate charge-exchange collisions of several isotopes for collision energies down to 400 neV (5 mK). The measured rate coefficient of $6 \times 10^{-10}$ cm$^{3}$s$^{-1}$, constant over four orders of magnitude in collision energy, is in good agreement with that derived from a semiclassical Langevin model for an atomic polarizability of 143 a.u.
A proposal for cooling the translational motion of optically levitated magnetic nanoparticles is presented. The theoretical cooling scheme involves the sympathetic cooling of a ferromagnetic YIG nanosphere with a spin-polarized atomic gas. Particle-atom cloud coupling is mediated through the magnetic dipole-dipole interaction. When the particle and atom oscillations are small compared to their separation, the interaction potential becomes dominantly linear which allows the particle to exchange energy with the $N$ atoms. While the atoms are continuously Doppler cooled, energy is able to be remo…
The potential energy curves, permanent and transition dipole moments, and the static dipolar polarizability, of molecular ions composed of one alkali-metal atom and a Strontium ion are determined with a quantum chemistry approach. The molecular ions are treated as effective two-electron systems and are treated using effective core potentials including core polarization, large gaussian basis sets, and full configuration interaction. In the perspective of upcoming experiments aiming at merging cold atom and cold ion traps, possible paths for radiative charge exchange, photoassociation of a cold …
Charge exchange X-ray emission provides unique insights into the interactions between cold and hot astrophysical plasmas. Besides its own profound science, this emission is also technically crucial to all observations in the X-ray band, since charge exchange with the solar wind often contributes a significant foreground component that contaminates the signal of interest. By approximating the cross sections resolved to $n$ and $l$ atomic subshells, and carrying out complete radiative cascade calculation, we create a new spectral code to evaluate the charge exchange emission in the X-ray band. C…
The role of electronic excitation in charge exchange chemical reactions between ultracold Ca atoms and Ba$^+$ ions, confined in a hybrid trap, is studied. This prototypical system is energetically precluded from reacting in its ground state, allowing a particularly simple interpretation of the influence of electronic excitation. It is found that while electronic excitation of the ion can critically influence the chemical reaction rate, electronic excitation of the neutral atom is less important. It is also experimentally demonstrated that with the correct choice of the atom-ion pair, it is pos…
We establish the existence of a fundamental limit to the efficiency of spin-exchange optical pumping of 3He nuclei by collisions with spin-polarized alkali-metal atoms. Using accurate ab initio calculations of molecular interactions and scattering properties, we show that the maximum 3He spin polarization that can be achieved in spin-exchange collisions with potassium (39K) and silver (107Ag) atoms is limited by the anisotropic hyperfine interaction. We find that spin exchange in Ag-He collisions occurs much faster than in K-He collisions, suggesting the possibility of using Ag in spin-exchang…
Atom-ion interactions occur through the electric dipole which is induced by the ion on the neutral atom. In a Langevin collision, in which the atom and ion overcome the centrifugal barrier and reach a short internuclear distance, their internal electronic states deform due to their interaction and can eventually alter. Here we explore the outcome products and the energy released from a single Langevin collision between a single cold $^{88}$Sr$^{+}$ ion initialized in the metastable $4d^2D_{5/2,3/2}$ states, and a cold $^{87}$Rb atom in the $5s^2S_{1/2}$ ground state. We found that the long-liv…
We study cold heteronuclear atom ion collisions by immersing a trapped single ion into an ultracold atomic cloud. Using ultracold atoms as reaction targets, our measurement is sensitive to elastic collisions with extremely small energy transfer. The observed energy-dependent elastic atom-ion scattering rate deviates significantly from the prediction of Langevin but is in full agreement with the quantum mechanical cross section. Additionally, we characterize inelastic collisions leading to chemical reactions at the single particle level and measure the energy-dependent reaction rate constants. …
Photoexcitation rates for creation of ultralong-range Rydberg molecules (ULRM) with 31$\lesssim n \lesssim41$ in both ground and excited vibrational levels in cold ($T\sim900$~nK) gases of polarized and unpolarized $^{87}$Sr are presented. The measured production rates of the $ν=0, 1$ and 2 vibrational levels reveal rather different $n$ dependences which are analyzed by evaluating the Franck-Condon factors associated with excitation of the different vibrational levels and molecular rotational states. In particular, for gases of spin-polarized fermions, only Rydberg dimers with odd rotational q…
A modified static exchange model is introduced, it could be useful to control the elastic s-wave scattering length in studying cold-atomic interaction. The theory includes the long-range van der Waals interaction in addition to short-range exchange force. The model is applied on Ps-H system to study the Feshbach resonances e.g. the s-wave elastic phase shifts and the corresponding cross sections at ultracold energies. These are compared with the data obtained using the static exchange model. A very interesting features are observed when we vary the interatomic separation i.e. the strength of d…
A mixed system of cooled and trapped, ions and atoms, paves the way for ion assisted cold chemistry and novel many body studies. Due to the different individual trapping mechanisms, trapped atoms are significantly colder than trapped ions, therefore in the combined system, the strong binary ion$-$atom interaction results in heat flow from ions to atoms. Conversely, trapped ions can also get collisionally heated by the cold atoms, making the resulting equilibrium between ions and atoms intriguing. Here we experimentally demonstrate, Rubidium ions (Rb$^+$) cool in contact with magneto-optically …
Atom-dimer exchange and dissociation reaction rates are predicted for different combinations of two $^4$He atoms and one of the alkaline species among $^{6}$Li, $^{7}$Li and $^{23}$Na, by using three-body scattering formalism with short-range two-body interactions. Our study was concerned with low-energy reaction rates in which the $s-$, $p-$ and $d-$ wave contributions are the relevant ones. The $^4$He is chosen as one of the atoms in the binary mixture, in view of previous available investigations and laboratory accessibilities. Focusing on possible experimental cold-atom realizations with t…
We investigate the prospects of controlling charge-exchange in ultracold collisions of heteroisotopic combinations of atoms and ions of the same element. The treatment, readily applicable to alkali or alkanine-earth metals, is illustrated in the process $^9$Be$^{+}$ + $^{10}$Be $\leftrightarrow$ $^{9}$Be + $^{10}$Be$^{+}$, which exhibits favorable electronic, nuclear, and hyperfine structure. Feshbach resonances are obtained from quantum scattering calculations in a standard coupled-channel formalism with non-BO terms originating from the nuclear kinetic operator. Near a narrow resonance predi…
We report a combined experimental and theoretical study of collision-induced dipolar relaxation in a cold spin-polarized gas of atomic nitrogen (N). We use buffer gas cooling to create trapped samples of 14N and 15N atoms with densities 5+/-2 x 10^{12} cm-3 and measure their magnetic relaxation rates at milli-Kelvin temperatures. Rigorous quantum scattering calculations based on accurate ab initio interaction potentials for the 7Sigma_u electronic state of N2 demonstrate that dipolar relaxation in N + N collisions occurs at a slow rate of ~10^{-13} cm3/s over a wide range of temperatures (1 mK…
Relevant uncertainties on theoretical atomic data are vital to determine the accuracy of plasma diagnostics in a number of areas including in particular the astrophysical study. We present a new calculation of the uncertainties on the present theoretical ion-impact charge exchange atomic data and X-ray spectra based on a set of comparisons with the existing laboratory data obtained in historical merged-beam, cold-target recoil-ion momentum spectroscopy, and electron beam ion traps experiments. The average systematic uncertainties are found to be 35-88% on the total cross sections, and 57-75% o…
Motivated by recent claims of a compelling ~3.5 keV emission line from nearby galaxies and galaxy clusters, we investigate a novel plasma model incorporating a charge exchange component obtained from theoretical scattering calculations. Fitting this kind of component with a standard thermal model yields positive residuals around 3.5 keV, produced mostly by S XVI transitions from principal quantum numbers n > 8 to the ground. Such high-n states can only be populated by the charge exchange process. In this scenario, the observed 3.5 keV line flux in clusters can be naturally explained by an inte…
Charge exchange (CX) is a semi-resonant recombination process that can lead to spectral line emission in the X-ray band. It occurs in nearly any environment where hot plasma and cold gas interact: in the solar system, in comets and planetary atmospheres, and likely astrophysically, in, for example, supernova remnants and galaxy clusters. It also contributes to the soft X-ray background. Accurate spectral modeling of CX is thus critical to properly interpreting our astrophysical observations, but the commonly used CX models in popular spectral fitting packages often rely on scaling equations an…
Charge exchange emission is known to provide a key diagnostic to the interface between hot and cold matter in many astrophysical environments. Most of the recent charge exchange studies focus on its emission in the X-ray band, but few on the UV part, although the latter can also provide a powerful probe of the charge exchange process. An atomic calculation, as well as an application to observed data, are presented to explore and describe the potential use of the UV data for the study of cosmic charge exchange. Using the newest charge exchange model in the SPEX code v3.03, we re-analyze an arch…
Charge exchange between highly charged ions and neutral atoms and molecules has been considered as one of the important mechanisms controlling soft X ray emissions in many astrophysical objects and environments. However, for modeling charge exchange soft X ray emission, the data of n and l resolved state selective capture cross sections are often obtained by empirical and semiclassical theory calculations. With a newly built cold target recoil ion momentum spectroscopy (COLTRIMS) apparatus, we perform a series of measurements of the charge exchange of Ne(8,9)+ ions with He and H2 for collision…
Though theoretically expected, the charge exchange emission from galaxy clusters has not yet been confidently detected. Accumulating hints were reported recently, including a rather marginal detection with the Hitomi data of the Perseus cluster. As suggested in Gu et al. (2015), a detection of charge exchange line emission from galaxy clusters would not only impact the interpretation of the newly-discovered 3.5 keV line, but also open up a new research topic on the interaction between hot and cold matter in clusters. We aim to perform the most systematic search for the O VIII charge exchange l…
