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Reactive Collisions and Interactions of Ultracold Dipolar Atoms

Svetlana Kotochigova

Published Oct 29, 2014• 0 citations
OpenAlex

Abstract

Abstract : We explored Feshbach resonances in the collision between ultracold highly-magnetic dysprosium and erbium atoms. The resonance density is orders of magnitude larger than seen in any other previously studied atomic system. Moreover, we showed that these resonance can only exist because of the anisotropic nature of the atom-atom potentials. Analysis of nearest-neighbor spacings between Feshbach resonances shows a chaotic distribution that one would expect from random-matrix theory. We explained these statistics as originating from the large strength of the anisotropy. We demonstrated that the vibrational motion of BaCl+ molecules is quenched by collisions with ultracold calcium atoms at a rate comparable to the Langevin rate. This is over four orders of magnitude more efficient than traditional sympathetic cooling schemes. In addition, we calculated the electronic structure of BaCl+ and other molecular ions. Based on these results we found unusually-large rates for cold charge-transfer reactions between neutral and ionic atoms.

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Inelastic Collisions and Chemical Reactions of Molecules at Ultracold Temperatures

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II. Inelastic atom -molecule collisions 2 A. Vibrational and rotational relaxation 2 1. Collisions at cold and ultracold temperatures 2 2. Shape resonances in molecular collisions 6 3. Feshbach resonances in molecular collisions 6 B. Quasi-resonant transitions 7 C. Atom -molecular ion collisions 8 III.Chemical Reactions at ultracold temperatures 9 A. Tunneling dominated reactions 9 1.Reactions at zero temperature 10 2. Feshbach resonances in reactive scattering 12 B. Barrierless reactions 14 1.Collision systems of three alkali metal atoms 14 2. Role of PES in determining ultracold reactions 16 3.Relaxation of vibrationally excited alkali metal dimers 18 4. Reactions of heteronuclear and isotopically substituted alkali-metal dimer systems 19 IV.Inelastic molecule -molecule collisions 20 A. Molecules in the ground vibrational state 20 B. Vibrationally inelastic transitions 22 V. Summary and outlook 24 References 24 I. A. Vibrational and rotational relaxation 1. Collisions at cold and ultracold temperatures

CRC Press eBooks•Jun 25, 2009•1 citation
Abstract : We explored Feshbach resonances in the collision between ultracold highly-magnetic dysprosium and erbium atoms. The resonance density is orders of magnitude larger than seen in any other previously studied atomic system. Moreover, we showed that these resonance can only exist because of the anisotropic nature of the atom-atom potentials. Analysis of nearest-neighbor spacings between Feshbach resonances shows a chaotic distribution that one would expect from random-matrix theory. We explained these statistics as originating from the large strength of the anisotropy. We demonstrated that the vibrational motion of BaCl+ molecules is quenched by collisions with ultracold calcium atoms at a rate comparable to the Langevin rate. This is over four orders of magnitude more efficient than traditional sympathetic cooling schemes. In addition, we calculated the electronic structure of BaCl+ and other molecular ions. Based on these results we found unusually-large rates for cold charge-transfer reactions between neutral and ionic atoms.
We show that for ultracold magnetic lanthanide atoms chaotic scattering emerges due to a combination of anisotropic interaction potentials and Zeeman coupling under an external magnetic field. This scattering is studied in a collaborative experimental and theoretical effort for both dysprosium and erbium. We present extensive atom-loss measurements of their dense magnetic Feshbach-resonance spectra, analyze their statistical properties, and compare to predictions from a random-matrix-theory-inspired model. Furthermore, theoretical coupled-channels simulations of the anisotropic molecular Hamiltonian at zero magnetic field show that weakly bound, near threshold diatomic levels form overlapping, uncoupled chaotic series that when combined are randomly distributed. The Zeeman interaction shifts and couples these levels, leading to a Feshbach spectrum of zero-energy bound states with nearest-neighbor spacings that changes from randomly to chaotically distributed for increasing magnetic field. Finally, we show that the extreme temperature sensitivity of a small, but sizable fraction of the resonances in the Dy and Er atom-loss spectra is due to resonant nonzero partial-wave collisions. Our threshold analysis for these resonances indicates a large collision-energy dependence of the three-body recombination rate.
This paper reviews current experimental and theoretical progress in the study of dipolar quantum gases of ground and meta-stable atoms with a large magnetic moment. We emphasize the anisotropic nature of Feshbach resonances due to coupling to fast-rotating resonant molecular states in ultracold s-wave collisions between magnetic atoms in external magnetic fields. The dramatic differences in the distribution of resonances of magnetic (7)S3 chromium and magnetic lanthanide atoms with a submerged 4f shell and non-zero electron angular momentum is analyzed. We focus on dysprosium and erbium as important experimental advances have been recently made to cool and create quantum-degenerate gases for these atoms. Finally, we describe progress in locating resonances in collisions of meta-stable magnetic atoms in electronic P-states with ground-state atoms, where an interplay between collisional anisotropies and spin-orbit coupling exists.
We explore collisions of atomic particles in two different regimes. In the first part of this work, we study atom-atom collisions of alkali metals at ultracold temperatures and conditions typically found in modern experiments. Feshbach resonances induced by external magnetic fields present a way to change collisional properties and exhibit control over cold collisions. We perform a fully quantum coupled-channel calculation in molecular orbital formalism to calculate collisional properties and characterize Feshbach resonances in ultracold Li+Na and Li+Rb systems. Furthermore, we use the results of these calculations as a foundation to propose a novel scheme for formation of stable ultracold molecules in their lowest rovibrational level. The formation scheme relies on the fact that the photoassociation rate becomes greatly enhanced in the vicinity of a Feshbach resonance, resulting in a large increase of the number of produced excited molecules. Efficient production of stable ultracold molecules is a prerequisite for realization of various proposed platforms for quantum computing with neutral atoms and molecules. In addition, we suggest a way to exploit specifics of the photoassociation rate behavior near its minimum for a precision measurement experiment to detect hypothetical variation of the electron-proton mass ratio in time. ^ The second part of this study examines ion-atom collisions in our solar system. Highly charged ions present in the solar wind collide with neutrals, capture one or more electrons into high excited states and deexcite, radiating energetic X-ray and UV photons. In particular, we study X-ray emissions charge-exchange collisions between fully stripped C6+, N7+ and O8+ solar wind ions and heliospheric hydrogen. We analytically solve the two-center Schrödinger equation and construct electronic potential curves for the aforementioned molecular ions. Subsequently, we compute polarization of the X-rays emitted in a single-step deexcitation following charge-exchange collisions and construct a polarization map for the ecliptic plane, as observed from Earth. Our analysis indicates that the heliospheric charge-exchange X-rays are slightly polarized, with the polarization P close to ten percent for the optimal line-of-sight. ^
Compared to purely atomic collisions, ultracold molecular collisions potentially support a much larger number of Fano-Feshbach resonances due to the enormous number of ro-vibrational states available. In fact, for alkali-metal dimers we find that the resulting density of resonances cannot be resolved at all, even on the sub-μμμK temperature scale of ultracold experiments. As a result, all observables become averaged over many resonances and can effectively be described by simpler, non-resonant scattering calculations. Two particular examples are discussed: non-chemically reactive RbCs and chemically reactive KRb. In the former case, the formation of a long-lived collision complex may lead to the ejection of molecules from a trap. In the latter case, chemical reactions broaden the resonances so much that they become unobservable.
We explore the anisotropic nature of Feshbach resonances in the collision between ultracold highly magnetic submerged-shell dysprosium atoms in their energetically lowest magnetic sublevel, which can only occur due to couplings to rotating bound states. This is in contrast to well-studied alkali-metal atom collisions, where broadest (strongest) Feshbach resonances are hyperfine induced and due to rotationless bound states. Our first-principle coupled-channel calculation of the collisions between these spin-polarized bosonic dysprosium atoms reveals a strong interplay between the anisotropies in the dispersion and magnetic dipole-dipole interaction. The former anisotropy is absent in alkali-metal and chromium collisions. We show that both types of anisotropy significantly affect the Feshbach spectrum as a function of an external magnetic field. Effects of the electrostatic quadrupole-quadrupole interaction are small. Over a 20 mT magnetic field range, we predict about 10 Feshbach resonances and show that the resonance locations depend on the dysprosium isotope.
II. Inelastic atom -molecule collisions 2 A. Vibrational and rotational relaxation 2 1. Collisions at cold and ultracold temperatures 2 2. Shape resonances in molecular collisions 6 3. Feshbach resonances in molecular collisions 6 B. Quasi-resonant transitions 7 C. Atom -molecular ion collisions 8 III.Chemical Reactions at ultracold temperatures 9 A. Tunneling dominated reactions 9 1.Reactions at zero temperature 10 2. Feshbach resonances in reactive scattering 12 B. Barrierless reactions 14 1.Collision systems of three alkali metal atoms 14 2. Role of PES in determining ultracold reactions 16 3.Relaxation of vibrationally excited alkali metal dimers 18 4. Reactions of heteronuclear and isotopically substituted alkali-metal dimer systems 19 IV.Inelastic molecule -molecule collisions 20 A. Molecules in the ground vibrational state 20 B. Vibrationally inelastic transitions 22 V. Summary and outlook 24 References 24 I. A. Vibrational and rotational relaxation 1. Collisions at cold and ultracold temperatures