Radiative decay processes at cold and ultra cold temperatures for Sulfur atoms colliding with protons are investigated. The MOLPRO quantum chemistry suite of codes was used to obtain accurate potential energies and transition dipole moments, as a function of internuclear distance, between low-lying states of the SH$^{+}$ molecular cation. A multi-reference configuration-interaction (MRCI) approximation together with the Davidson correction is used to determine the potential energy curves and transition dipole moments, between the states of interest, where the molecular orbitals (MO's) are obtained from state-averaged multi configuration-self-consistent field (MCSCF) calculations. The collision problem is solved approximately using an optical potential method to obtain radiative loss, and a fully two-channel quantum approach for radiative charge transfer. Cross sections and rate coefficients are determined for the first time for temperatures ranging from 10 $μ$ K up to 10,000 K. Results are obtained for all isotopes of Sulfur, colliding with H$^{+}$ and D$^{+}$ ions and comparison is made to a number of other collision systems.
We use the quantum threshold laws combined with a classical capture model to provide an analytical estimate of the chemical quenching cross sections and rate coefficients of two colliding particles at ultralow temperatures. We apply this quantum threshold model (QT model) to indistinguishable fermionic polar molecules in an electric field. At ultracold temperatures and in weak electric fields, the cross sections and rate coefficients depend only weakly on the electric dipole moment d induced by the electric field. In stronger electric fields, the quenching processes scale as d^{4(L+1/2)} where…
The control of the ultracold collisions between neutral atoms is an extensive and successful field of study. The tools developed allow for ultracold chemical reactions to be managed using magnetic fields, light fields and spin-state manipulation of the colliding particles among other methods. The control of chemical reactions in ultracold atom-ion collisions is a young and growing field of research. Recently, the collision energy and the ion electronic state were used to control atom-ion interactions. Here, we demonstrate spin-controlled atom-ion inelastic processes. In our experiment, both sp…
We report scattering lengths for the singlet Sigma g +, triplet Sigma u + and quintet Sigma g + adiabatic molecular potentials relevant to collisions of two metastable (n=2 triplet S) helium atoms as a function of the uncertainty in these potentials. These scattering lengths are used to calculate experimentally observable scattering lengths, elastic cross sections and inelastic rates for any combination of states of the colliding atoms, at temperatures where the Wigner threshold approximation is valid.
Ultracold collisions of cold atoms or molecules make the bound states of the collision complex formed from the two colliding species accessible for control and manipulation of the cold species or the complex. Such resonances are best treated by a resonant scattering theory, which in the ultracold domain can take advantage of the properties of the long-range potential and the methods of multichannel quantum defect theory. Coupled channels calculations on the threshold scattering states and bound states of the 40K87Rb molecule illustrate the ideas and methodology of quantum defect theory using t…
We report on three-body recombination of a single trapped Rb^+ ion and two neutral Rb atoms in an ultracold atom cloud. We observe that the corresponding rate coefficient K_3 depends on collision energy and is about a factor of 1000 larger than for three colliding neutral Rb atoms. In the three-body recombination process large energies up to several 0.1eV are released leading to an ejection of the ion from the atom cloud. It is sympathetically recooled back into the cloud via elastic binary collisions with cold atoms. Further, we find that the final ionic product of the three-body processes is…
Scattering and ionizing cross sections and rates are calculated for ultracold collisions between metastable helium atoms using a fully quantum-mechanical close-coupled formalism. Homonuclear collisions of the bosonic ${}^{4}$He$^{*} +{}^{4}$He$^{*}$ and fermionic ${}^{3}$He$^{*} + {}^{3}$He$^{*}$ systems, and heteronuclear collisions of the mixed ${}^{3}$He$^{*} +{}^{4}$He$^{*}$ system, are investigated over a temperature range 1 $μ$K to 1 K. Carefully constructed Born-Oppenheimer molecular potentials are used to describe the electrostatic interaction between the colliding atoms, and complex o…
Progress in ultracold experiments with polar molecules requires a clear understanding of their interactions and reactivity at ultra-low collisional energies. Two important theoretical steps in this process are the characterization of interaction potentials between molecules and the modeling of reactive scattering mechanism. Here, we report on the {\it abinitio} calculation of isotropic and anisotropic van der Waals interaction potentials for polar KRb and RbCs colliding with each other or with ultracold atoms. Based on these potentials and two short-range scattering parameters we then develop …
We discuss the production of ultracold molecules in their electronic ground state by photoassociation employing electronically excited states with ion-pair character and strong spin-orbit interaction. A short photoassociation laser pulse drives a non-resonant three-photon transition for alkali atoms colliding in their lowest triplet state. The excited state wave packet is transferred to the ground electronic state by a second laser pulse, driving a resonant two-photon transition. After analyzing the transition matrix elements governing the stabilization step, we discuss the efficiency of popul…
Ultracold atomic gases have realised numerous paradigms of condensed matter physics where control over interactions has crucially been afforded by tunable Feshbach resonances. So far, the characterisation of these Feshbach resonances has almost exclusively relied on experiments in the threshold regime near zero energy. Here we use a laser-based collider to probe a narrow magnetic Feshbach resonance of rubidium above threshold. By measuring the overall atomic loss from colliding clouds as a function of magnetic field, we track the energy-dependent resonance position. At higher energy, our colli…
We extent the recently developed Multi-Layer Multi-Configuration Time-Dependent Hartree method for Bosons (ML-MCTDHB) for simulating the correlated quantum dynamics of bosonic mixtures to the fermionic sector and establish a unifying approach for the investigation of the correlated quantum dynamics of mixture of indistinguishable particles, be it fermions or bosons. Relying on a multi-layer wave-function expansion, the resulting Multi-Layer Multi-Configuration Time-Dependent Hartree method for Mixtures (ML-MCTDHX) can be adapted to efficiently resolve system-specific intra- and inter-species c…
We develop the theory for the Adiabatic Raman Photoassociation (ARPA) of ultracold atoms to form ultracold molecules in the presence of scattering resonances. Based on a computational method in which we replace the continuum with a discrete set of "effective modes", we show that the existence of resonances greatly aids in the formation of deeply bound molecular states. We illustrate our general theory by computationally studying the formation of $^{85}$Rb$_2$ molecules from pairs of colliding ultracold $^{85}$Rb atoms. The single-event transfer yield is shown to have a near-unity value for wid…
We observe light-induced frequency shifts in one-color photoassociative spectra of magnetically trapped $^4$He$^*$ atoms in the metastable $2^3S_1$ state. A pair of ultracold spin-polarized $2^3S_1$ helium atoms is excited into a molecular bound state in the purely long range $0_u^+$ potential connected to the $2^3S_1 - 2^3P_0$ asymptote. The shift arises from the optical coupling of the molecular excited bound state with the scattering states and the bound states of two colliding $2^3S_1$ atoms. We measure the frequency-shifts for several ro-vibrational levels in the $0^+_u$ potential and fin…
We analyze a system of two colliding ultracold atoms under strong harmonic confinement from the viewpoint of quantum defect theory and formulate a generalized self-consistent method for determining the allowed energies. We also present two highly efficient computational methods for determining the bound state energies and eigenfunctions of such systems. The perturbed harmonic oscillator problem is characterized by a long asymptotic region beyond the effective range of the interatomic potential. The first method, which is based on quantum defect theory and is an adaptation of a technique develo…
We investigate confinement-induced resonances in a system composed by a tightly trapped ion and a moving atom in a waveguide. We determine the conditions for the appearance of such resonances in a broad region -- from the "long-wavelength" limit to the opposite case when the typical length scale of the atom-ion polarisation potential essentially exceeds the transverse waveguide width. We find considerable dependence of the resonance position on the atomic mass which, however, disappears in the "long-wavelength and zero-energy" limit, where the known result for the confined atom-atom scattering…
Most of the current theories on the p-wave superfluid in cold atomic gases are based on the effective-range theory for the two-body scattering, where the low energy p-wave scattering amplitude $f_1(k)$ is given by $% f_1(k)=-1/[ik+1/(\mathcal{V}k^2)+1/\mathcal{R}]$, where $k$ is the incident momentum, and $\mathcal{V}$ and $\mathcal{R}$ are the $k$-independent scattering volume and effective-range, respectively. However, due to the long-range nature of the van der Waals interaction between two colliding ultracold atoms, the p-wave scattering amplitude of the two atoms is not described by the e…
We report on calculations of the elastic cross section and thermalization rate for collision between two maximally spin-polarized chromium atoms in the cold and ultracold regimes, relevant to buffer-gas and magneto-optical cooling of chromium atoms. We calculate ab initio potential energy curves for Cr2 and the van der Waals coefficient C6, and construct interaction potentials between two colliding Cr atoms. We explore the effect of shape resonances on elastic cross section, and find that they dramatically affect the thermalization rate. Our calculated value for the s-wave scattering length is…
Chemical reaction rates often depend strongly on stereodynamics, namely the orientation and movement of molecules in three-dimensional space. An ultracold molecular gas, with a temperature below 1 uK, provides a highly unusual regime for chemistry, where polar molecules can easily be oriented using an external electric field and where, moreover, the motion of two colliding molecules is strictly quantized. Recently, atom-exchange reactions were observed in a trapped ultracold gas of KRb molecules. In an external electric field, these exothermic and barrierless bimolecular reactions, KRb+KRb -> …
Elastic scattering cross sections are measured for lithium atoms colliding with rare gas atoms and SF6 molecules at tunable relative velocities down to ~50 m/s. Our scattering apparatus combines a velocity-tunable molecular beam with a magneto-optic trap that provides an ultracold cloud of lithium atoms as a scattering target. Comparison with theory reveals the quantum nature of the collision dynamics in the studied regime, including both rainbows as well as orbiting resonances.
We present quantum-theoretical studies of collisions between an open-shell S-state atom and a ^2Pi-state molecule in the presence of a magnetic field. We analyze the collisional Hamiltonian and discuss possible mechanisms for inelastic collisions in such systems. The theory is applied to the collisions of the nitrogen atom (^4S) with the OH molecule, with both collision partners initially in fully spin-stretched (magnetically trappable) states, assuming that the interaction takes place exclusively on the two high-spin (quintet) potential energy surfaces. The surfaces for the quintet states are…
We demonstrate that it is possible to efficiently control ultracold chemical reactions of alkali-metal atoms colliding with open-shell alkali-metal dimers in their metastable triplet states by choosing the internal hyperfine and rovibrational states of the reactants as well as by inducing magnetic Feshbach resonances with an external magnetic field. We base these conclusions on coupled-channel statistical calculations that include the effects of hyperfine contact and magnetic-field-induced Zeeman interactions on ultracold chemical reactions of hyperfine-resolved ground-state Na and the triplet…
We present a joint experimental and theoretical study of spin dynamics of a single $^{88}$Sr$^+$ ion colliding with an ultracold cloud of Rb atoms in various hyperfine states. While spin-exchange between the two species occurs after 9.1(6) Langevin collisions on average, spin-relaxation of the Sr$^+$ ion Zeeman qubit occurs after 48(7) Langevin collisions which is significantly slower than in previously studied systems due to a small second-order spin-orbit coupling. Furthermore, a reduction of the endothermic spin-exchange rate was observed as the magnetic field was increased. Interestingly, …
We investigate the possibility of forming deeply bound ultracold RbCs molecules by a two-color photoassociation experiment. We compare the results with those for Rb_2 in order to understand the characteristic differences between heteronuclear and homonuclear molecules. The major differences arise from the different long-range potential for excited states. Ultracold 85Rb and 133Cs atoms colliding on the X^1Sigma+ potential curve are initially photoassociated to form excited RbCs molecules in the region below the Rb(5S) + Cs(6P_1/2) asymptote. We explore the nature of the Omega=0^+ levels in thi…
We report on the study of binary collisions between quantum droplets formed by an attractive mixture of ultracold atoms. We distinguish two main outcomes of the collision, i.e. merging and separation, depending on the velocity of the colliding pair. The critical velocity $v_c$ that discriminates between the two cases displays a different dependence on the atom number $N$ for small and large droplets. By comparing our experimental results with numerical simulations, we show that the non-monotonic behavior of $v_c(N)$ is due to the crossover from a compressible to an incompressible regime, where…
We model the dynamics of attractively interacting ultracold bosonic atoms in a quasi-one-dimensional wave-guide with additional harmonic trapping. Initially, we prepare the system in its ground state and then shift the zero of the harmonic trap and switch on an additional narrow scattering potential near the center of the trap. After colliding with the barrier twice, we propose to measure the number of atoms opposite to the initial condition. Quantum-enhanced interferometry with quantum bright solitons allows us to predict detection of an offset of the scattering potential with considerably in…
