arXiv subjects

Jeremy M. Hutson

Publications and source records attributed to Jeremy M. Hutson.

At least 109 records · Page 6Linked to original sources

arXiv2012

Multichannel Quantum Defect Theory for cold molecular collisions with a strongly anisotropic potential energy surface

We show that multichannel quantum defect theory (MQDT) can be applied successfully as an efficient computational method for cold molecular collisions in Li+NH, which has a deep and strongly anisotropic interaction potential. In this strongly coupled system, closed-channel poles restrict the range over which the MQDT Y matrix can be interpolated. We present an improved procedure to transform the MQDT reference functions so that the poles are removed from the energy range of interest. Effects due to very long-range spin-dipolar couplings are outside the scope of MQDT, but can be added perturbatively. The new procedure makes it possible to calculate the elastic and inelastic cross sections needed to evaluate the feasibility of sympathetic cooling of NH by Li using coupled-channel calculations at only 5 combinations of energy and field.

physics.chem-ph↗

arXiv2012

Feshbach spectroscopy of an ultracold mixture of $^{85}$Rb and $^{133}$Cs

We report the observation of interspecies Feshbach resonances in an optically trapped mixture of $^{85}$Rb and $^{133}$Cs. We measure 14 interspecies features in the lowest spin channels for a magnetic field range from 0 to 700 G and show that they are in good agreement with coupled-channel calculations. The interspecies background scattering length is close to zero over a large range of magnetic fields, permitting the sensitive detection of Feshbach resonances through interspecies thermalisation. Our results confirm the quality of the Rb-Cs potential curves and offer promising starting points for the production of ultracold polar molecules.

physics.atom-ph↗

arXiv2012

Optimized Multichannel Quantum Defect Theory for cold molecular collisions

Multichannel quantum defect theory (MQDT) can provide an efficient alternative to full coupled-channel calculations for low-energy molecular collisions. However, the efficiency relies on interpolation of the Y matrix that encapsulates the short-range dynamics, and there are poles in Y that may prevent interpolation over the range of energies of interest for cold molecular collisions. We show how the phases of the MQDT reference functions may be chosen so as to remove such poles from the vicinity of a reference energy and dramatically increase the range of interpolation. For the test case of Mg+NH, the resulting optimized Y matrix may be interpolated smoothly over an energy range of several Kelvin and a magnetic field range of over 1000 G. Calculations at additional energies and fields can then be performed at a computational cost that is proportional to the number of channels N and not to N^3.

physics.chem-ph↗

arXiv2012

Towards the production of ultracold ground-state RbCs molecules: Feshbach resonances, weakly bound states, and coupled-channel model

We have studied interspecies scattering in an ultracold mixture of $^{87}$Rb and $^{133}$Cs atoms, both in their lowest-energy spin states. The three-body loss signatures of 30 incoming s- and p-wave magnetic Feshbach resonances over the range 0 to 667 G have been catalogued. Magnetic field modulation spectroscopy was used to observe molecular states bound by up to 2.5 MHz$\times h$. Magnetic moment spectroscopy along the magneto-association pathway from 197 to 182 G gives results consistent with the observed and calculated dependence of the binding energy on magnetic field strength. We have created RbCs Feshbach molecules using two of the resonances. We have set up a coupled-channel model of the interaction and have used direct least-squares fitting to refine its parameters to fit the experimental results from the Feshbach molecules, in addition to the Feshbach resonance positions and the spectroscopic results for deeply bound levels. The final model gives a good description of all the experimental results and predicts a large resonance near 790 G, which may be useful for tuning the interspecies scattering properties. Quantum numbers and vibrational wavefunctions from the model can also be used to choose optimal initial states of Feshbach molecules for their transfer to the rovibronic ground state using stimulated Raman adiabatic passage (STIRAP).

physics.atom-ph↗

arXiv2011

Magnetically tunable Feshbach resonances in ultracold Li-Yb mixtures

We investigate the possibility of forming Li+Yb ultracold molecules by magnetoassociation in mixtures of ultracold atoms. We find that magnetically tunable Feshbach resonances exist, but are extremely narrow for even-mass ytterbium isotopes, which all have zero spin. For odd-mass Yb isotopes, however, there is a new mechanism due to hyperfine coupling between the electron spin and the Yb nuclear magnetic moment. This mechanism produces Feshbach resonances for fermionic Yb isotopes that can be more than 2 orders of magnitude larger than for the bosonic counterparts.

physics.atom-ph↗

arXiv2011

Optically induced conical intersections in traps for ultracold atoms and molecules

We show that conical intersections can be created in laboratory coordinates by dressing a parabolic trap for ultracold atoms or molecules with a combination of optical and static magnetic fields. The resulting ring trap can support single-particle states with half-integer rotational quantization and many-particle states with persistent flow. Two well-separated atomic or molecular states are brought into near-resonance by an optical field and tuned across each other with an inhomogeneous magnetic field. Conical intersections occur at the nodes in the optical field.

cond-mat.quant-gas↗

arXiv2011

Multichannel Quantum Defect Theory for cold molecular collisions

Multichannel Quantum Defect Theory (MQDT) is shown to be capable of producing quantitatively accurate results for low-energy atom-molecule scattering calculations. With a suitable choice of reference potential and short-range matching distance, it is possible to define a matrix that encapsulates the short-range collision dynamics and is only weakly dependent on energy and magnetic field. Once this has been produced, calculations at additional energies and fields can be performed at a computational cost that is proportional to the number of channels N and not to N^3. MQDT thus provides a promising method for carrying out low-energy molecular scattering calculations on systems where full exploration of the energy- and field-dependence is currently impractical.

physics.atom-ph↗

arXiv2011

The effect of hyperfine interactions on ultracold molecular collisions: NH(^3Sigma^-) with Mg(^1S) in magnetic fields

We investigate the effect of hyperfine interactions on ultracold molecular collisions in magnetic fields, using ^{24}Mg(^1S) + ^{14}NH(^3Sigma^-) as a prototype system. We explore the energy and magnetic field dependence of the cross sections, comparing the results with previous calculations that neglected hyperfine interactions (Phys. Rev. Lett. 103, 183201 (2009)). The main effect of hyperfine interactions for spin relaxation cross sections is that the kinetic energy release of the dominant outgoing channels does not reduce to zero at low fields. This results in reduced centrifugal suppression on the cross sections and increased inelastic cross sections at low energy and low field. We also analyze state-to-state cross sections, for various initial states, and show that hyperfine interactions introduce additional mechanisms for spin relaxation. In particular, there are hyperfine-mediated collisions to outgoing channels that are not centrifugally suppressed. However, for Mg+NH these unsuppressed channels make only small contributions to the total cross sections. We consider the implications of our results for sympathetic cooling of NH by Mg and conclude that the ratio of elastic to inelastic cross sections remains high enough for sympathetic cooling to proceed.

physics.chem-ph↗

arXiv2011

Cold collisions of an open-shell S-state atom with a ^2Pi molecule: N(^4S) colliding with OH in a magnetic field

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 obtained from spin-unrestricted coupled-cluster calculations with single, double, and noniterative triple excitations. We find substantial inelasticity, arising from strong couplings due to the anisotropy of the interaction potential and the anisotropic spin-spin dipolar interaction. The mechanism involving the dipolar interaction dominates for small magnetic field strengths and ultralow collision energies, while the mechanism involving the potential anisotropy prevails when the field strength is larger (above 100 G) or the collision energy is higher (above 1 mK). The numerical results suggest that sympathetic cooling of magnetically trapped OH by collisions with ultracold N atoms will not be successful at higher temperatures.

physics.chem-ph↗

arXiv2011

Cold and ultracold NH--NH collisions: The field-free case

We present elastic and inelastic spin-changing cross sections for cold and ultracold NH($X\,^3Σ^-$) + NH($X\,^3Σ^-$) collisions, obtained from full quantum scattering calculations on an accurate \textit{ab initio} quintet potential-energy surface. Although we consider only collisions in zero field, we focus on the cross sections relevant for magnetic trapping experiments. It is shown that evaporative cooling of both fermionic $^{14}$NH and bosonic $^{15}$NH is likely to be successful for hyperfine states that allow for s-wave collisions. The calculated cross sections are very sensitive to the details of the interaction potential, due to the presence of (quasi-)bound state resonances. The remaining inaccuracy of the \textit{ab initio} potential-energy surface therefore gives rise to an uncertainty in the numerical cross-section values. However, based on a sampling of the uncertainty range of the \textit{ab initio} calculations, we conclude that the exact potential is likely to be such that the elastic-to-inelastic cross-section ratio is sufficiently large to achieve efficient evaporative cooling. This likelihood is only weakly dependent on the size of the channel basis set used in the scattering calculations.

physics.chem-ph↗

arXiv2011

Prospects for sympathetic cooling of molecules in electrostatic, ac and microwave traps

We consider how trapped molecules can be sympathetically cooled by ultracold atoms. As a prototypical system, we study LiH molecules co-trapped with ultracold Li atoms. We calculate the elastic and inelastic collision cross sections of LiH + Li with the molecules initially in the ground state and in the first rotationally excited state. We then use these cross sections to simulate sympathetic cooling in a static electric trap, an ac electric trap, and a microwave trap. In the static trap we find that inelastic losses are too great for cooling to be feasible for this system. The ac and microwave traps confine ground-state molecules, and so inelastic losses are suppressed. However, collisions in the ac trap can take molecules from stable trajectories to unstable ones and so sympathetic cooling is accompanied by trap loss. In the microwave trap there are no such losses and sympathetic cooling should be possible.

physics.atom-ph↗

arXiv2011

The prospects of sympathetic cooling of NH molecules with Li atoms

We calculate the quartet potential energy surface for Li+NH and use it to calculate elastic and spin-relaxation cross sections for collisions in magnetically trappable spin-stretched states. The potential is strongly anisotropic but spin-relaxation collisions are still suppressed by centrifugal barriers when both species are in spin-stretched states. In the ultracold regime, both the elastic and inelastic cross sections fluctuate dramatically as the potential is varied because of Feshbach resonances. The potential-dependence is considerably reduced at higher energies. The major effect of using an unconverged basis set in the scattering calculations is to shift the resonances without changing their general behaviour. We have calculated the ratio of elastic and spin-relaxation cross sections, as a function of collision energy and magnetic field, for a variety of potential energy surfaces. Most of the surfaces produce ratios that are favorable for sympathetic cooling, at temperatures below about 20 mK.

physics.atom-ph↗

arXiv2011

Interaction between LiH molecule and Li atom from state-of-the-art electronic structure calculations

State-of-the-art ab initio techniques have been applied to compute the potential energy surface for the lithium atom interacting with the lithium hydride molecule in the Born-Oppenheimer approximation. The interaction potential was obtained using a combination of the explicitly correlated unrestricted coupled-cluster method with single, double, and noniterative triple excitations [UCCSD(T)-F12] for the core-core and core-valence correlation and full configuration interaction for the valence-valence correlation. The potential energy surface has a global minimum 8743 cm^{-1} deep if the Li-H bond length is held fixed at the monomer equilibrium distance or 8825 cm^{-1} deep if it is allowed to vary. In order to evaluate the performance of the conventional CCSD(T) approach, calculations were carried out using correlation-consistent polarized valence X-tuple-zeta bases, with X ranging from 2 to 5. The contribution beyond the CCSD(T)-F12 model, obtained from full configuration interaction (FCI) calculations for the valence-valence correlation, was shown to be very small. At linear LiH-Li geometries the ground-state potential shows an avoided crossing with an ion-pair potential.Using both adiabatic and diabatic pictures we analyse the interaction between the two potential energy surfaces and its possible impact on the collisional dynamics. When the LiH bond is allowed to vary, a seam of conical intersections appears at C_{2v} geometries. At the linear LiH-Li geometry, the conical intersection is at a Li-H distance which is only slightly larger than the monomer equilibrium distance, but for nonlinear geometries it quickly shifts to Li-H distances that are well outside the classical turning points of the ground-state potential of LiH. Finally, the reaction channels for the exchange and insertion reactions are also analyzed.

physics.chem-ph↗

arXiv2010

Cold and ultracold NH--NH collisions in magnetic fields

Elastic and spin-changing inelastic collision cross sections are presented for cold and ultracold magnetically trapped NH. The cross sections are obtained from coupled-channel scattering calculations as a function of energy and magnetic field. We specifically investigate the influence of the intramolecular spin-spin, spin-rotation, and intermolecular magnetic dipole coupling on the collision dynamics. It is shown that $^{15}$NH is a very suitable candidate for evaporative cooling experiments. The dominant trap-loss mechanism in the ultracold regime originates from the intermolecular dipolar coupling term. At higher energies and fields, intramolecular spin-spin coupling becomes increasingly important. Our qualitative results and conclusions are fairly independent of the exact form of the potential and of the size of the channel basis set.

physics.chem-ph↗

arXiv2010

Cold collisions of N atoms and NH molecules in magnetic fields

We calculate the interaction potential between N atoms and NH molecules and use it to investigate cold and ultracold collisions important for sympathetic cooling. The ratio of elastic to inelastic cross sections is large over a wide range of collision energy and magnetic field for most isotopic combinations, so that sympathetic cooling of NH molecules by N atoms is a good prospect. However, there are important effects due to a p-wave shape resonance that may inhibit cooling in some cases. We show that scaling the reduced mass used in the collision is approximately equivalent to scaling the interaction potential. We then explore the dependence of the scattering properties on the reduced mass and explain the resonant effects observed using angular-momentum-insensitive quantum defect theory

physics.chem-ph↗

arXiv2010

Ultracold RbSr molecules can be formed by magnetoassociation

We investigate the interactions between ultracold alkali metal atoms and closed-shell atoms using electronic structure calculations on the prototype system Rb+Sr. There are molecular bound states that can be tuned across atomic thresholds with magnetic field, and there are previously neglected terms in the collision Hamiltonian that can produce zero-energy Feshbach resonances with significant widths. The largest effect comes from the interaction-induced variation of the Rb hyperfine coupling. The resonances may be used to form paramagnetic polar molecules if the magnetic field can be controlled precisely enough.

physics.atom-ph↗

arXiv2010

Reactions of ultracold alkali metal dimers

We investigate the energetics of reactions involving pairs of alkali metal dimers. Atom exchange reactions to form homonuclear dimers are energetically allowed for some but not all of the heteronuclear dimers. We carry out high-level electronic structure calculations on the potential energy surfaces of all the heteronuclear alkali metal trimers and show that trimer formation reactions are always energetically forbidden for low-lying singlet states of the dimers. The results have important implications for the stability of quantum gases of alkali metal dimers.

physics.atom-ph↗

arXiv2009

Quantum gas of rovibronic ground-state molecules in an optical lattice

Control over all internal and external degrees of freedom of molecules at the level of single quantum states will enable a series of fundamental studies in physics and chemistry. In particular, samples of ground-state molecules at ultralow temperatures and high number densities will allow novel quantum-gas studies and future applications in quantum information science. However, high phase-space densities for molecular samples are not readily attainable as efficient cooling techniques such as laser cooling are lacking. Here we produce an ultracold and dense sample of molecules in a single hyperfine level of the rovibronic ground state with each molecule individually trapped in the motional ground state of an optical lattice well. Starting from a zero-temperature atomic Mott-insulator state with optimized double-site occupancy, weakly-bound dimer molecules are efficiently associated on a Feshbach resonance and subsequently transferred to the rovibronic ground state by a stimulated four-photon process with >50 % efficiency. The molecules are trapped in the lattice and have a lifetime of 8 s. Our results present a crucial step towards Bose-Einstein condensation of ground-state molecules and, when suitably generalized to polar heteronuclear molecules, the realization of dipolar quantum-gas phases in optical lattices.

cond-mat.quant-gas↗