We propose a new method for the production of ultracold molecular ions. This method utilizes sympathetic cooling due to the strong collisions between appropriately chosen molecular ions and laser-cooled neutral atoms to realize ultracold, internal ground-state molecular ions. In contrast to other experiments producing cold molecular ions, our proposed method efficiently cools both the internal and external molecular ion degrees of freedom. The availability of an ultracold, absolute ground-state sample of molecular ions would have broad impact to fields as diverse as quantum chemistry, astrophysics, and fundamental physics; and may lead to the development of a robust, scalable quantum computer.
We report the trapping of ultracold neutral $ \text{Rb}$ atoms and $ \text{Ba}^+ $ ions in a common optical potential in absence of any radiofrequency (RF) fields. We prepare $ \text{Ba}^+ $ at $ 370 ~ μK $ and demonstrate efficient sympathetic cooling by $100 ~ μK $ after one collision. Our approach is currently limited by the $ \text{Rb}$ density and related three-body losses, but it overcomes the fundamental limitation in RF traps set by RF-driven, micromotion-induced heating. It is applicable to a wide range of ion-atom species, and may enable novel ultracold chemistry experiments and comp…
The formation of $^{40}$Ca$_2^+$ molecular ions is observed in a hybrid $^{40}$Ca magneto-optical and ion trap system. The molecular ion formation process is determined to be two-photon photo-associative ionization of ultracold $^{40}$Ca atoms. A lower bound for the two-body, two-photon rate constant is found to be $\barβ \geq 2 \pm 1 \times 10^{-15}$ cm$^{3}$ Hz. $\textit{Ab initio}$ molecular potential curves are calculated for the neutral Ca$_2$ and ionic Ca$_2^+$ molecules and used in a model that identifies the photo-associative ionization pathway. As this technique does not require a sep…
Charge exchange collisions between ultracold fermionic 6Li atoms and 40Ca+ ions are observed in the mK temperature range. The reaction product of the charge exchange collision is identified via mass spectrometry during which the motion of the ions is excited parametrically. The cross-sections of the charge exchange collisions between 6Li atoms in the ground state and 40Ca+ ions in the ground and metastable excited states are determined. Investigation of the inelastic collision characteristics in the atom-ion mixture is an important step toward ultracold chemistry based on ultracold atoms and i…
We describe a hybrid vacuum system in which a single ion or a well defined small number of trapped ions (in our case Ba$^+$ or Rb$^+$) can be immersed into a cloud of ultracold neutral atoms (in our case Rb). This apparatus allows for the study of collisions and interactions between atoms and ions in the ultracold regime. Our setup is a combination of a Bose-Einstein condensation (BEC) apparatus and a linear Paul trap. The main design feature of the apparatus is to first separate the production locations for the ion and the ultracold atoms and then to bring the two species together. This schem…
The Ca$^+$, Sr$^+$, Ba$^+$, and Yb$^+$ ions immersed in an ultracold gas of the Cr atoms are proposed as experimentally feasible heteronuclear systems in which ion-atom interactions at ultralow temperatures can be controlled with magnetically tunable Feshbach resonances without charge transfer and radiative losses. \textit{Ab initio} techniques are applied to investigate electronic-ground-state properties of the (CaCr)$^+$, (SrCr)$^+$, (BaCr)$^+$, and (YbCr)$^+$ molecular ions. The potential energy curves, permanent electric dipole moments, and static electric dipole polarizabilities are compu…
We estimate the radiative quenching rate of the $^{40}$Ca - $^{174}$Yb$^{+}$ molecular ion and find that it under-estimates the value reported in recent experiments by about 5 orders of magnitude. We comment on possible explanations for this large discrepancy.
We theoretically study trapped ions that are immersed in an ultracold gas of Rydberg-dressed atoms. By off-resonant coupling on a dipole-forbidden transition, the adiabatic atom-ion potential can be made repulsive. We study the energy exchange between the atoms and a single trapped ion and find that Langevin collisions are inhibited in the ultracold regime for these repulsive interactions. Therefore, the proposed system avoids recently observed ion heating in hybrid atom-ion systems caused by coupling to the ion's radio frequency trapping field and retains ultracold temperatures even in the pr…
We are developing a new hybrid atom-ion trap to study the interaction of ultracold rubidium atoms with mass-selected OH- molecules. The ions are trapped inside an octupole rf-trap made of thin wires instead of the commonly used rods. This ensures good optical access to the center of the trap where the ions can be overlapped with laser cooled rubidium atoms stored in a dark spontaneous force optical trap (dark SPOT). This setup provides high collision rates since the density in a dark SPOT is about one order of magnitude higher than in a standard magneto-optical trap. Further, inelastic collisi…
The two most widely used ion cooling methods are laser cooling and sympathetic cooling by elastic collisions (ECs). Here we demonstrate another method of cooling ions that is based on resonant charge exchange (RCE) between the trapped ion and the ultracold parent atom. Specifically, trapped Cs$^{+}$ ions are cooled by collisions with co-trapped, ultracold Cs atoms and, separately, by collisions with co-trapped, ultracold Rb atoms. We observe that the cooling of Cs$^{+}$ ions by Cs atoms is more efficient than cooling of Cs$^{+}$ ions by Rb atoms. This signals the presence of a cooling mechanis…
For exploration of quantum effects with hybrid atom-ion systems, reaching ultracold temperatures is the major limiting factor. In this work, we present results on numerical simulations of trapped ion buffer gas cooling using an ultracold atomic gas in a large number of experimentally realistic scenarios. We explore the suppression of micromotion-induced heating effects through optimization of trap parameters for various radio-frequency (rf) traps and rf driving schemes including linear and octupole traps, digital Paul traps, rotating traps and hybrid optical/rf traps. We find that very similar…
Experiments with cold ion-atom mixtures have recently opened the way for the production and application of ultracold molecular ions. Here, in a comparative study, we theoretically investigate ground and several excited electronic states and prospects for the formation of molecular ions composed of a calcium ion and an alkali-metal atom: CaAlk$^{+}$ (Alk=Li, Na, K, Rb, Cs). We use a quantum chemistry approach based on non-empirical pseudopotential, operatorial core-valence correlation, large Gaussian basis sets, and full configuration interaction method for valence electrons. Adiabatic potentia…
We report on the observation of interactions between ultracold Rydberg atoms and ions in a Paul trap. The rate of observed inelastic collisions, which manifest themselves as charge transfer between the Rydberg atoms and ions, exceeds that of Langevin collisions for ground state atoms by about three orders of magnitude. This indicates a huge increase in interaction strength. We study the effect of the vacant Paul trap's electric fields on the Rydberg excitation spectra. To quantitatively describe the exhibited shape of the ion loss spectra, we need to include the ion-induced Stark shift on the …
Experimental setups that study laser-cooled ions immersed in baths of ultracold atoms merge the two exciting and well-established fields of quantum gases and trapped ions. These experiments benefit both from the exquisite read-out and control of the few-body ion systems as well as the many-body aspects, tunable interactions, and ultracold temperatures of the atoms. However, combining the two leads to challenges both in the experimental design and the physics that can be studied. Nevertheless, these systems have provided insights into ion-atom collisions, buffer gas cooling of ions and quantum …
We present a scheme to embed molecular anions in a gas of ultracold rubidium atoms as a route towards the preparation of cold molecular ions by collisional cooling with ultracold atoms. Associative detachment as an important loss process in collisions between OH- molecules and rubidium atoms is studied. The density distribution of trapped negative ions in the multipole radiofrequency trap is measured by photodetachment tomography, which allows us to derive absolute rate coefficients for the process. We define a regime where translational and internal cooling of molecular ions embedded into the…
We present an experimental scheme which combines the well established method of velocity-mapimaging, with a cold trapped metastable neon target. The device is used for obtaining the branching ratios and recoil-ion energy distributions for the penning ionization process in optical collisions of ultracold metastable neon. The potential depth of the highly excited dimer potential is extracted and compared with theoretical calculations. The simplicity to construct, characterize and apply such a device, makes it a unique tool for the low-energy nuclear physics community, enabling opportunities for …
Interactions between cold ions and atoms have been proposed for use in implementing quantum gates\cite{Idziaszek2007}, probing quantum gases\cite{Sherkunov2009}, observing novel charge-transport dynamics\cite{Cote2000}, and sympathetically cooling atomic and molecular systems which cannot be laser cooled\cite{Smith2005,Hudson2009}. Furthermore, the chemistry between cold ions and atoms is foundational to issues in modern astrophysics, including the formation of stars, planets, and interstellar clouds\cite{Smith1992}, the diffuse interstellar bands\cite{Reddy2010}, and the post-recombination ep…
We measure chemical reactions between a single trapped $^{174}$Yb$^+$ ion immersed in an ultracold bath of $^6$Li atoms containing trace amounts of Li$_2$ dimers. This produces LiYb$^+$ molecular ions that we detect via mass spectrometry. We explain the reaction rates by modelling the dimer density as a function of the magnetic field and obtain excellent agreement when we assume the reaction to follow the Langevin rate. Our results present a novel approach towards the creation of cold molecular ions and point to the exploration of ultracold chemistry in ion molecule collisions. What is more, w…
We investigate the energy dependence and the internal-state dependence of the charge-exchange collision cross sections in a mixture of $^6$Li atoms and $^{40}$Ca$^+$ ions in the collision energy range from 0.2 mK to 1 K. Deliberately excited ion micromotion is used to control the collision energy of atoms and ions. The energy dependence of the charge-exchange collision cross section obeys the Langevin model in the temperature range of the current experiment, and the measured magnitude of the cross section is correlated to the internal state of the $^{40}$Ca$^+$ ions. Revealing the relationship…
In order to study ultracold charge-transfer processes in hybrid atom-ion traps, we have mapped out the potential energy curves and molecular parameters for several low lying states of the Rb, Yb$^+$ system. We employ both a multi-reference configuration interaction (MRCI) and a full configuration interaction (FCI) approach. Turning points, crossing points, potential minima and spectroscopic molecular constants are obtained for the lowest five molecular states. Long-range parameters, including the dispersion coefficients are estimated from our {\it ab initio} data. The separated-atom ionization…
We experimentally demonstrate cooling of trapped ions by collisions with co-trapped, higher mass neutral atoms. It is shown that the lighter $^{39}$K$^{+}$ ions, created by ionizing $^{39}$K atoms in a magneto-optical trap (MOT), when trapped in an ion trap and subsequently allowed to cool by collisions with ultracold, heavier $^{85}$Rb atoms in a MOT, exhibit a longer trap lifetime than without the localized $^{85}$Rb MOT atoms. A similar cooling of trapped $^{85}$Rb$^{+}$ ions by ultracold $^{133}$Cs atoms in a MOT is also demonstrated in a different experimental configuration to validate th…
We have generated Coulomb crystals of ultracold $^4$He$^+$ ions in a linear radiofrequency trap, by sympathetic cooling via laser--cooled $^9$Be$^+$. Stable crystals containing up to 150 localized He$^+$ ions at $\sim$20 mK were obtained. Ensembles or single ultracold He$^+$ ions open up interesting perspectives for performing precision tests of QED and measurements of nuclear radii. The present work also indicates the feasibility of cooling and crystallizing highly charged atomic ions using $^9$Be$^+$ as coolant.
We report optical absorption imaging of ultracold neutral plasmas.Images are used to measure the ion absorption spectrum, which is Doppler-broadened. Through the spectral width, we monitor ion equilibration in the first 250ns after plasma formation. The equilibration leaves ions on the border between the weakly coupled gaseous and strongly coupled liquid states. On a longer timescale of microseconds, we observe radial acceleration of ions resulting from pressure exerted by the trapped electron gas.
We report a detailed molecular spectroscopy study on the lowest excited electronic states of $^{23}\rm{Na}^{87}\rm{Rb}$ for producing ultracold $^{23}\rm{Na}^{87}\rm{Rb}$ molecules in the electronic, rovibrational and hyperfine ground state. Starting from weakly-bound Feshbach molecules, a series of vibrational levels of the $A^{1}Σ^{+}-b^{3}Π$ coupled excited states were investigated. After resolving, modeling and interpreting the hyperfine structure of several lines, we successfully identified a long-lived level resulting from the accidental hyperfine coupling between the $0^+$ and $0^-$ com…
We have realized a high-resolution time-of-flight mass spectrometer combined with a magneto-optical trap. The spectrometer enables excellent optical access to the trapped atomic cloud using specifically devised acceleration and deflection electrodes. The ions are extracted along a laser beam axis and deflected onto an off axis detector. The setup is applied to detect atoms and molecules photoassociated from ultracold atoms. The detection is based on resonance-enhanced multi-photon ionization. Mass resolution up to m/Delta m_rms = 1000 at the mass of 133Cs is achieved. The performance of this s…
We report the creation of an ultracold neutral plasma by photoionization of laser-cooled xenon atoms. The charge carrier density is as high as 2 x 10^9 cm^-3, and the temperatures of electrons and ions are as low as 100 mK and 10 uK, respectively. Plasma behavior is evident in the trapping of electrons by the positive ion cloud when the Debye screening length becomes smaller than the size of the sample. We produce plasmas with parameters such that both electrons and ions are strongly coupled.
Ion-atom interactions are a comparatively recent field of research that has drawn considerable attention due to its applications in areas including quantum chemistry and quantum simulations. In first experiments, atomic ions and neutral atoms have been successfully overlapped by devising hybrid apparatuses combining established trapping methods, Paul traps for ions and optical or magneto-optical traps for neutral atoms, respectively. Since then, the field has seen considerable progress, but the inherent presence of radiofrequency (rf) fields in such hybrid traps was found to have a limiting im…
Controlling physical systems and their dynamics on the level of individual quanta propels both fundamental science and quantum technologies. Trapped atomic and molecular systems, neutral and charged, are at the forefront of quantum science. Their extraordinary level of control is evidenced by numerous applications in quantum information processing and quantum metrology. Studying the long-range interactions between these systems when combined in a hybrid atom-ion trap has lead to landmark results. Reaching the ultracold regime, however, where quantum mechanics dominates the interaction, e.g., g…
We describe a hybrid molecular dynamics approach for the description of ultracold neutral plasmas, based on an adiabatic treatment of the electron gas and a full molecular dynamics simulation of the ions, which allows us to follow the long-time evolution of the plasma including the effect of the strongly coupled ion motion. The plasma shows a rather complex relaxation behavior, connected with temporal as well as spatial oscillations of the ion temperature. Furthermore, additional laser cooling of the ions during the plasma evolution drastically modifies the expansion dynamics, so that crystall…
While ion heating by elastic electron-ion collisions may be neglected for a description of the evolution of freely expanding ultracold neutral plasmas, the situation is different in scenarios where the ions are laser-cooled during the system evolution. We show that electron-ion collisions in laser-cooled plasmas influence the ionic temperature, decreasing the degree of correlation obtainable in such systems. However, taking into account the collisions increases the ion temperature much less than what would be estimated based on static plasma clouds neglecting the plasma expansion. The latter l…
A versatile apparatus for simultaneous trapping of multiple species of ultracold atoms and ions to enable studies of low energy collisions and cold chemistry
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 on a measurement of the characteristic temperature of an ultracold rubidium ion source, in which a cloud of laser-cooled atoms is converted to ions by photo-ionization. Extracted ion pulses are focused on a detector with a pulsed-field technique. The resulting experimental spot sizes are compared to particle-tracking simulations, from which a source temperature $T = (1 \pm 2)$ mK and the corresponding transversal reduced emittance $ε_r = 7.9 X 10^{-9}$ m rad $\sqrt{\rm{eV}}$ are determined. We find that this result is likely limited by space charge forces even though the average numb…
Experimental realizations of charged ions and neutral atoms in overlapping traps are gaining increasing interest due to their wide research application ranging from chemistry at the quantum level to quantum simulations of solid-state systems. Here, we describe a system in which we overlap a single ground-state cooled ion trapped in a linear Paul trap with a cloud of ultracold atoms such that both constituents are in the $μ$K regime. Excess micromotion (EMM) currently limits atom-ion interaction energy to the mK energy scale and above. We demonstrate spectroscopy methods and compensation techni…
We report the spontaneous formation of a plasma from a gas of cold Rydberg molecules. Double-resonant laser excitation promotes nitric oxide, cooled to 1 K in a seeded supersonic molecular beam, to single Rydberg states extending as deep as 80 cm$^{-1}$ below the lowest ionization threshold. The density of excited molecules in the illuminated volume is as high as 1 x 10$^{13}$ cm$^{-3}$. This population evolves to produce prompt free electrons and a durable cold plasma of electrons and intact NO$^{+}$ ions.
Hybrid systems of laser-cooled trapped ions and ultracold atoms combined in a single experimental setup have recently emerged as a new platform for fundamental research in quantum physics. This paper reviews the theoretical and experimental progress in research on cold hybrid ion-atom systems which aim to combine the best features of the two well-established fields. We provide a broad overview of the theoretical description of ion-atom mixtures and their applications, and report on advances in experiments with ions trapped in Paul or dipole traps overlapped with a cloud of cold atoms, and with…
Molecular ions formed in cold hybrid ion-atom experiments may find interesting applications ranging from precision measurements to controlled chemical reactions. Here, we investigate electronic structure of the Sr$_2^+$ molecular ion, which may be produced by photoassociation of laser-cooled Sr$^+$ ions immersed into an ultracold gas of Sr atoms or by ionization of ultracold Sr$_2$ molecules. Using \textit{ab initio} electronic structure methods, such as the coupled cluster and configuration interaction ones with small-core relativistic energy-consistent pseudopotentials and large Gaussian bas…
Spontaneous avalanche to plasma splits the core of an ellipsoidal Rydberg gas of nitric oxide. Ambipolar expansion first quenches the electron temperature of this core plasma. Then, long-range, resonant charge transfer from ballistic ions to frozen Rydberg molecules in the wings of the ellipsoid quenches the centre-of-mass ion/Rydberg molecule velocity distribution. This sequence of steps gives rise to a remarkable mechanics of self-assembly, in which the kinetic energy of initially formed hot electrons and ions drives an observed separation of plasma volumes. These dynamics adiabatically sequ…
In this chapter we review the progress in experiments with hybrid systems of trapped ions and ultracold neutral atoms. We give a theoretical overview over the atom-ion interactions in the cold regime and give a summary of the most important experimental results. We conclude with an overview of remaining open challenges and possible applications in hybrid quantum systems of ions and neutral atoms.
We present a study of vibrational quenching and chemical processes of molecular ions immersed in an ultracold atomic gas by means of the quasi-classical trajectory (QCT) method. In particular, BaRb$^+(v)$ + Rb collisions are studied at cold temperatures revealing a highly efficient energy transfer between the translational degrees of freedom and internal degrees of the molecular ion. Thus leading to a large vibrational quenching cross section which follows the Langevin capture model prediction. These results play a key role on the understanding of relaxation phenomena of cold molecular ions in…
Hybrid quantum systems that unite laser-cooled trapped ions and ultracold quantum gases in a single experimental setup have opened a rapidly advancing field of study, including Quantum chemistry, polaron physics, quantum information processing and quantum simulations. We present a fully developed and tested ion trap chip and propose a flat chip trap that can be placed beneath the ion trap. This design substantially addresses the difficulties specific to hybrid traps and features well-aligned chips that allow for independent adjustment of the depth of the atomic trap and the confinement and pos…
We consider the possibilities for producing ultracold mixtures of K and Cs and forming KCs molecules by magnetoassociation. We carry out coupled-channel calculations of the interspecies scattering length for $^{39}$KCs, $^{41}$KCs and $^{40}$KCs and characterize Feshbach resonances due to s-wave and d-wave bound states, with widths ranging from below 1 nG to 5 G. We also calculate the corresponding bound-state energies as a function of magnetic field. We give a general discussion of the combinations of intraspecies and interspecies scattering lengths needed to form low-temperature atomic mixtu…
Chemical reactions can be surprisingly efficient at ultracold temperatures ( < 1mK) due to the wave nature of atoms and molecules. The study of reactions in the ultracold regime is a new research frontier enabled by cooling and trapping techniques developed in atomic and molecular physics. In addition, ultracold molecular gases that offer diverse molecular internal states and large electric dipolar interactions are sought after for studies of strongly interacting many-body quantum physics. Here we propose a new approach for producing ultracold molecules in the absolute internal and motional qu…
We have suggested a method for treating different quantum few-body dynamics without usual partial-wave analysis. With this approach new results were obtained in the physics of ultracold atom-atom collisions and ionization and excitation/deexitation of helium ions. The developed computational scheme opens new possibilities for analysis the actual problem of ultracold atom wave-packets collisions in strong laser or magnetic confinement.
It has been roughly three decades since laser cooling techniques produced ultracold atoms, leading to rapid advances in a vast array of fields. Unfortunately laser cooling has not yet been extended to molecules because of their complex internal structure. However, this complexity makes molecules potentially useful for many applications. For example, heteronuclear molecules possess permanent electric dipole moments which lead to long-range, tunable, anisotropic dipole-dipole interactions. The combination of the dipole-dipole interaction and the precise control over molecular degrees of freedom …
We present a theoretical analysis of optical pathways for formation of cold Ca($^1$S)Na$^+$($^1$S) molecular ions via an intermediate state. The formation schemes are based on ab initio potential energy curves and transition dipole moments calculated using effective-core-potential methods of quantum chemistry. In the proposed approach, starting from a mixture of cold trapped Ca$^+$ ions immersed into an ultracold gas of Na atoms, (NaCa)$^+$ molecular ions are photoassociated in the excited E$^{1}Σ^+$ electronic state and allowed to spontaneously decay either to the ground electronic state or a…
We theoretically study the dynamics of a trapped ion that is immersed in an ultracold gas of weakly bound atomic dimers created by a Feshbach resonance. Using quasi-classical simulations, we find a crossover from dimer dissociation to molecular ion formation depending on the binding energy of the dimers. The location of the crossover strongly depends on the collision energy and the time-dependent fields of the Paul trap. Deeply bound dimers lead to fast molecular ion formation, with rates approaching the Langevin collision rate $Γ'_\text{L}\approx4.8\times10^{-9}\,$cm$^3$s$^{-1}$. The kinetic …
We demonstrate a simple technique for molecular ion spectroscopy. BaCl$^+$ molecular ions are trapped in a linear Paul trap in the presence of a room-temperature He buffer gas and photodissociated by driving an electronic transition from the ground X$^1Σ^+$ state to the repulsive wall of the A$^1Π$ state. The photodissociation spectrum is recorded by monitoring the induced trap loss of BaCl$^+$ ions as a function of excitation wavelength. Accurate molecular potentials and spectroscopic constants are determined. Comparison of the theoretical photodissociation cross-sections with the measurement…
We argue that the quenched ultracold plasma presents an experimental platform for studying quantum many-body physics of disordered systems in the long-time and finite energy-density limits. We consider an experiment that quenches a plasma of nitric oxide to an ultracold system of Rydberg molecules, ions and electrons that exhibits a long-lived state of arrested relaxation. The qualitative features of this state fail to conform with classical models. Here, we develop a microscopic quantum description for the arrested phase based on an effective many-body spin Hamiltonian that includes both dipo…
There is substantial interest in producing samples of ultracold molecules for possible applications in quantum computation, quantum simulation of condensed matter systems, precision measurements, controlled chemistry, and high precision spectroscopy. A crucial step to obtaining large samples of ultracold, trapped molecules is developing a means to bridge the gap between typical molecular source velocities (~150-600 m/s) and velocities for which trap loading or confinement is possible (~5-20 m/s). Here we show deceleration of a beam of neutral strontium monofluoride (SrF) molecules using radiat…
We present a new quantum gas apparatus for ultracold mixtures of K and Cs atoms and ultracold samples of KCs ground-state molecules. We demonstrate the apparatus' capabilities by producing Bose-Einstein condensates (BEC) of 39K and 133Cs in a manner that will eventually allow sequential condensation within one experimental cycle, precise sample overlap, and magnetic association of atoms into KCs molecules. The condensates are created independently without relying on sympathetic cooling. Our approach is universal and applicable to other species combinations when the two species show dramaticall…
