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arXiv:1301.5518

Shedding Light on Three-Body Recombination in an Ultracold Atomic Gas

Arne Härter, Artjom Krükow, Markus Deiß, Björn Drews, E. Tiemann, Johannes Hecker Denschlag

Published Jan 23, 2013• 5 citations
arXivHTMLPDF

Abstract

Three-body recombination is a prime example of the fundamental interaction between three particles. Due to the complexity of this process it has resisted a comprehensive description. Experimental investigations have mainly focussed on the observation of corresponding loss rates without revealing information on the reaction products. Here, we provide the first general experimental study on the population distribution of molecular quantum states after three-body recombination in a non-resonant regime. We have developed a highly sensitive detection scheme which combines photoionization of the molecules with subsequent ion trapping. By analyzing the ionization spectrum, we identify the population of energy levels with binding energies up to $h\times 750\:$GHz. We find a broad population of electronic and nuclear spin states and determine a range of populated vibrational and rotational states. The method presented here can be expanded to provide a full survey of the products of the recombination process. This may be pivotal in developing an in-depth model that can qualitatively and quantitatively predict the reaction products of three-body recombination.

DOI
10.48550/arxiv.1301.5518

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Three-body recombination is a prime example of the fundamental interaction between three particles. Due to the complexity of this process it has resisted a comprehensive description. Experimental investigations have mainly focussed on the observation of corresponding loss rates without revealing information on the reaction products. Here, we provide the first general experimental study on the population distribution of molecular quantum states after three-body recombination in a non-resonant regime. We have developed a highly sensitive detection scheme which combines photoionization of the molecules with subsequent ion trapping. By analyzing the ionization spectrum, we identify the population of energy levels with binding energies up to h×750 h\times 750\:h×750GHz. We find a broad population of electronic and nuclear spin states and determine a range of populated vibrational and rotational states. The method presented here can be expanded to provide a full survey of the products of the recombination process. This may be pivotal in developing an in-depth model that can qualitatively and quantitatively predict the reaction products of three-body recombination.
In this thesis, I report on experiments on the detection and the production of molecules in an ultracold atomic gas. These experiments can be divided into two main parts. The first part is about state-to-state experiments where chemical reaction products are detected in a quantum state resolved way. The second part is about Rydberg molecules. In the first part, I investigate three-body recombination of neutral Rb, which is a chemical reaction leading to the formation of Rb2 dimers. The quantum states of the three-body recombination product molecules are investigated for different initial atomic samples. This includes different atomic hyperfine states and different atomic magnetic sub states that are prepared. The molecular reaction product is state-selectively ionized and detected afterwards. The detection scheme resolves total electron spin, the vibrational, the rotational, the hyperfine and even the magnetic sub state of the product molecules. We determine the population distribution of the product molecules covering the majority of all produced molecules. The insights gained enable us to formulate various propensity rules for the three-body recombination of 87Rb. The second part is furthermore divided into two parts: the investigations of charged and uncharged Rydberg molecules. The investigations of charged Rydberg molecules are the first step towards one of our goals, the photoassociation of BaRb+ or Rb2+ Rydberg molecules. For this work, we have developed a novel method to measure Stark spectra within an ion trap. In experiments with neutral Rb2 Rydberg molecules we observe a complex spin structure of the molecular states. The substructure emerges partially due to a novel, recently predicted spin-orbit interaction of the Rydberg electron and the perturber atom, which we prove for the first time.
Three-body recombination is a chemical reaction where the collision of three atoms leads to the formation of a diatomic molecule. In the ultracold regime it is expected that the production rate of a molecule generally decreases with its binding energy Eb{E}_{b}Eb​, however, its precise dependence and the physics governing it have been left unclear so far. Here we present a comprehensive experimental and theoretical study of the energy dependency for three-body recombination of ultracold Rb. For this, we determine production rates for molecules in a state-to-state resolved manner, with the binding energies Eb{E}_{b}Eb​ ranging from 0.02 to 77 $\mathrm{GHz}\ifmmode\times\else\texttimes\fi{}h$. We find that the formation rate approximately scales as ${E}_{b}^{\ensuremath{-}\ensuremath{\alpha}}$, where $\ensuremath{\alpha}$ is in the vicinity of 1. The formation rate typically varies only within a factor of two for different rotational angular momenta of the molecular product, apart from a possible centrifugal barrier suppression for low binding energies. In addition to numerical three-body calculations we present a perturbative model which reveals the physical origin of the energy scaling of the formation rate. Furthermore, we show that the scaling law potentially holds universally for a broad range of interaction potentials.
Three-body recombination is a chemical reaction where the collision of three atoms leads to the formation of a diatomic molecule. In the ultracold regime it is expected that the production rate of a molecule generally decreases with its binding energy Eb, however, its precise dependence and the physics governing it have been left unclear so far. Here we present a comprehensive experimental and theoretical study of the energy dependency for three-body recombination of ultracold Rb. For this, we determine production rates for molecules in a state-to-state resolved manner, with the binding energies Eb ranging from 0.02 to 77 GHz×h. We find that the formation rate approximately scales as Eb-α, where α is in the vicinity of 1. The formation rate typically varies only within a factor of two for different rotational angular momenta of the molecular product, apart from a possible centrifugal barrier suppression for low binding energies. In addition to numerical three-body calculations we present a perturbative model which reveals the physical origin of the energy scaling of the formation rate. Furthermore, we show that the scaling law potentially holds universally for a broad range of interaction potentials.
During the last few decades, the two fields of ultracold neutral atoms and of single trapped ions have undergone an amazing development. The incorporation of these systems into a single experiment exploits the complementary physical properties of the subsystems and opens up novel lines of research. I present experimental results obtained in one of the first hybrid atom-ion setups accessing the cold regime. Single ions interact with ultracold samples of 87Rb atoms. The collision energies are set by heating mechanisms in the Paul trap and are on the order of mK·kB. Interactions are generally strong and long-ranged. We observe elastic atom-ion scattering in the semi-classical energy regime in which the cross section depends on the collision energy and favors scattering at small angles. We were able to obtain a general good understanding of atom-ion two-body collisions. We observed sympathetic cooling of the ion over four orders of magnitude in energy through collisions with the ultracold atoms. Further, we utilized atom-ion scattering events to develop a novel method to compensate excess ion micromotion, the primary source of ion heating. Three-body collisions between two atoms and the ion play an important role. We identified these processes through the large amounts of energy that they release. This makes them detectable despite their suppression with respect to two-body collisions. We also showed that atom-ion three-body collisions become more prominent as the collision energy decreases. Finally, we employed our atom-ion apparatus to gain novel insights into three-body recombination between ultracold atoms. In these experiments the ion trap acts as an extremely sensitive ion detector. Through three-body recombination a Rb2 molecule is formed and can undergo ionization by absorbing photons from a strong laser. By scanning the frequency of the ionization laser we obtained a molecular spectrum and identified a relatively broad distribution over final molecular states.
We are developing theoretical and computational methods to study two related three-body processes in ultracold quantum gases: three-body resonances and three-body recombination. Three-body recombination causes the ultracold gas to heat up and atoms to leave the trap where they are confined. Therefore, it is an undesirable effect in the process of forming ultracold quantum gases. Metastable three-body states (resonances) are formed in the ultracold gas. When decaying they also give additional kinetic energy to the gas, that leads to the heating too. In addition, a reliable method to obtain three-body resonances would be useful in a number of problems in other fields of physics, for example, in models of metastable nuclei or to study dissociative recombination of H3 +. Our project consists of employing computer modeling to develop a method to obtain three-body resonances. The method uses a novel two-step diagonalization approach to solve the three-body Schrödinger equation. The approach employs the SVD method of Tolstikhin et al. coupled with a complex absorbing potential. We tested this method on a model system of three identical bosons with nucleon mass and compared it to the results of a previous study. This model can be employed to understand the 3He nucleus . We found one three-body bound state and four resonances. We are also studying Efimov resonances using a 4He-based model. In a system of identical spinless bosons, Efimov states are a series of loosely bound three-body states which begin to appear as the energy of the two-body bound state approaches zero . Although they were predicted 35 years ago, recent evidence of Efimov states found by Kraemer et al. in a gas of ultracold Cs atoms has sparked great interest by theorists and experimentalists. Efimov resonances are a kind of pre-dissociated Efimov trimer. To search for Efimov resonances we tune the diatom interaction potential, V(r): V(r) → λV(r) as Esry et al. did . We calculated the first two values of λ for which there is a "condensation" (infinite number) of Efimov states. They are λEfimov1 = 0.9765 and λEfimov2 = 6.834. We performed calculations for λ = 2.4, but found no evidence of Efimov resonances. For future work we plan to work with λ ≈ 4 and λ ≈ λEfimov2 where we might see d-wave and higher l-wave Efimov resonances. There is also a many-body project that forms part of this thesis and consists of a direct diagonalization of the Bogolyubov Hamiltonian, which describes elementary excitations of a gas of bosons interacting through a pairwise interaction. We would like to reproduce the corresponding energy spectrum. So far we have performed several convergence tests, but have not observed the desired energy spectrum. We show preliminary results.
We propose a platform for observing and controlling the interactions between atomic ions and a quantum gas of polar molecules in the ultracold regime. This approach is based on the combination of several recently developed methods in two so-far complementary research domains: ion-atom collisions and studies of ultracold polar molecules. In contrast to collisions between ions and ground-state atoms, which are dominated by losses due to three-body recombination (TBR) already at densities far below those typical for quantum degenerate ensembles, our proposal makes use of polar molecules, their rich level structure, and sensitivity to electric fields to design effective interaction potentials where ion-neutral TBR losses and molecule-molecule losses due to sticky collisions could be strongly suppressed. This may open a broad range of applications including precise control of collisional properties in molecular ensembles using ions, quantum simulations, and cold quantum chemistry between polyatomic molecules.