Rotational predissociation of extremely weakly bound atom-molecule complexes produced by Feshbach resonance association

We study the rotational predissociation of atom - molecule complexes with very small binding energy. Such complexes can be produced by Feshbach resonance association of ultracold molecules with ultracold atoms. Numerical calculations of the predissociation lifetimes based on the computation of the energy dependence of the scattering matrix elements become inaccurate when the binding energy is smaller than the energy width of the predissociating state. We derive expressions that represent accurately the predissociation lifetimes in terms of the real and imaginary parts of the scattering length and effective range for molecules in an excited rotational state. Our results show that the predissociation lifetimes are the longest when the binding energy is positive, i.e. when the predissociating state is just above the excited state threshold.Comment: 17 pages, 5 figure

Three-State Feshbach Resonances Mediated By Second-Order Couplings

We present an analytical study of three-state Feshbach resonances induced by second-order couplings. Such resonances arise when the scattering amplitude is modified by the interaction with a bound state that is not directly coupled to the scattering state containing incoming flux. Coupling occurs indirectly through an intermediate state. We consider two problems: (i) the intermediate state is a scattering state in a distinct open channel; (ii) the intermediate state is an off-resonant bound state in a distinct closed channel. The first problem is a model of electric-field-induced resonances in ultracold collisions of alkali metal atoms [Phys. Rev. A 75, 032709 (2007)] and the second problem is relevant for ultracold collisions of complex polyatomic molecules, chemical reaction dynamics, photoassociation of ultracold atoms, and electron - molecule scattering. Our analysis yields general expressions for the energy dependence of the T-matrix elements modified by three-state resonances and the dependence of the resonance positions and widths on coupling amplitudes for the weak-coupling limit. We show that the second problem can be generalized to describe resonances induced by indirect coupling through an arbitrary number of sequentially coupled off-resonant bound states and analyze the dependence of the resonance width on the number of the intermediate states.Comment: 27 pages, 4 figures; added a reference; journal reference/DOI refer to final published version, which is a shortened and modified version of this preprin

Vibrational energy transfer in ultracold molecule - molecule collisions

We present a rigorous study of vibrational relaxation in p-H2 + p-H2 collisions at cold and ultracold temperatures and identify an efficient mechanism of ro-vibrational energy transfer. If the colliding molecules are in different rotational and vibrational levels, the internal energy may be transferred between the molecules through an extremely state-selective process involving simultaneous conservation of internal energy and total rotational angular momentum. The same transition in collisions of distinguishable molecules corresponds to the rotational energy transfer from one vibrational state of the colliding molecules to another.Comment: 4 pages, 4 figure

Total angular momentum representation for atom-molecule collisions in electric fields

It is shown that the atom-molecule collision problem in the presence of an external electric field can be solved using the total angular momentum representation in the body-fixed coordinated frame, leading to a computationally efficient method for ab initio modeling of low-temperature scattering phenomena. Our calculations demonstrate rapid convergence of the cross sections for vibrational and Stark relaxation in He-CaD collisions with the number of total angular momentum states in the basis set, leading to a 5-100 fold increase in computational efficiency over the previously used methods based on the fully uncoupled space-fixed representation. These results open up the possibility of carrying out numerically converged quantum scattering calculations on a wide array of atom-molecule collisions and chemical reactions in the presence of electric fields.Comment: 19 pages, 3 figures, 1 tabl

Predicting and verifying transition strengths from weakly bound molecules

We investigated transition strengths from ultracold weakly bound 41K87Rb molecules produced via the photoassociation of laser-cooled atoms. An accurate potential energy curve of the excited state (3)1Sigma+ was constructed by carrying out direct potential fit analysis of rotational spectra obtained via depletion spectroscopy. Vibrational energies and rotational constants extracted from the depletion spectra of v'=41-50 levels were combined with the results of the previous spectroscopic study, and they were used for modifying an ab initio potential. An accuracy of 0.14% in vibrational level spacing and 0.3% in rotational constants was sufficient to predict the large observed variation in transition strengths among the vibrational levels. Our results show that transition strengths from weakly bound molecules are a good measure of the accuracy of an excited state potential.Comment: 7 pages, 7 figure

Coherent transfer of photoassociated molecules into the rovibrational ground state

We report on the direct conversion of laser-cooled 41K and 87Rb atoms into ultracold 41K87Rb molecules in the rovibrational ground state via photoassociation followed by stimulated Raman adiabatic passage. High-resolution spectroscopy based on the coherent transfer revealed the hyperfine structure of weakly bound molecules in an unexplored region. Our results show that a rovibrationally pure sample of ultracold ground-state molecules is achieved via the all-optical association of laser-cooled atoms, opening possibilities to coherently manipulate a wide variety of molecules.Comment: 4 pages, 4 figure

Loss of molecules in magneto-electrostatic traps due to nonadiabatic transitions

We analyze the dynamics of a paramagnetic, dipolar molecule in a generic "magneto-electrostatic'' trap where both magnetic and electric fields may be present. The potential energy that governs the dynamics of the molecules is found using a reduced molecular model that incorporates the main features of the system. We discuss the shape of the trapping potentials for different field geometries, as well as the possibility of nonadiabatic transitions to untrapped states, i.e., the analog of Majorana transitions in a quadrupole magnetic atomic trap. Maximizing the lifetime of molecules in a trap is of great concern in current experiments, and we assess the effect of nonadiabatic transitions on obtainable trap lifetimes.Comment: 13 pages, 6 figure

Channel Electron Multiplier and Channelplate Efficiencies for Detecting Positive Ions

Absolute detection efficiencies for singly and multiply charged positive ions have been measured for a channelplate and for two different channel electron multipliers (CEM). The efficiencies were measured for impact energies between approximately 0.25 and 25 keV and for ion masses ranging from 14 to 132. The maximum efficiencies were found to be the same for all ions investigated and were approximately 58% for a channelplate and 89% for the CEMs. For a channelplate it is shown that the detection efficiencies for heavier ions scale to a single curve if plotted versus the impact energy divided by the square root of the ion mass. Data taken from the literature imply that lighter ions scale differently. Polynomial fitting parameters to the present efficiency curves are provided

Cold and Slow Molecular Beam

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 10^9 molecules per pulse. The other has the slowest forward velocity of vf = 40 m/s, a longitudinal temperature of 3.6 K, and a flux of 5x10^8 molecules per pulse