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Nature Physics

Population distribution of product states following three-body recombination in an ultracold atomic gas

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

Published Jun 23, 2013• 65 citations
Publisher
DOI
10.1038/nphys2661

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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.

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Atom-atom-anion three-body recombination (TBR) in mixed 4He and xLi− (x = 6 or 7) is investigated in the adiabatic hyperspherical representation by quantum mechanically solving the Schrödinger equation. The distributions of product states following these TBR processes are found to be relatively different for the two systems when the collision energy is less than roughly 0.6 mK × kB or 0.3 mK × kB for 4He4He6Li− and 4He4He7Li− systems, respectively, with kB being the Boltzmann constant. For 4He4He6Li− systems, the rate of recombination into (v=0) l = 04He6Li− molecular anions is the largest with v and l denoting the rovibrational quantum numbers, while the TBR rate that leads to the formation of l = 14He6Li− molecular anions is a little smaller than that of neutral 4He2 molecules. For 4He4He7Li− systems, neutral 4He2 molecules tend to be the most products, following the yields of l = 0 and 1 4He7Li− molecular anions. However, in spite of these distinctly different distributions, the products of molecular anions, the sum of l = 0 and 1 4HexLi− products, are relatively larger than that of neutral 4He2 molecules for both the two systems.

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Final state distribution in three-body recombination of three ultracold 87^{87}87Rb atoms
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.
Atom-atom-anion three-body recombination (TBR) in mixed 4He and xLi− (x = 6 or 7) is investigated in the adiabatic hyperspherical representation by quantum mechanically solving the Schrödinger equation. The distributions of product states following these TBR processes are found to be relatively different for the two systems when the collision energy is less than roughly 0.6 mK × kB or 0.3 mK × kB for 4He4He6Li− and 4He4He7Li− systems, respectively, with kB being the Boltzmann constant. For 4He4He6Li− systems, the rate of recombination into (v=0) l = 04He6Li− molecular anions is the largest with v and l denoting the rovibrational quantum numbers, while the TBR rate that leads to the formation of l = 14He6Li− molecular anions is a little smaller than that of neutral 4He2 molecules. For 4He4He7Li− systems, neutral 4He2 molecules tend to be the most products, following the yields of l = 0 and 1 4He7Li− molecular anions. However, in spite of these distinctly different distributions, the products of molecular anions, the sum of l = 0 and 1 4HexLi− products, are relatively larger than that of neutral 4He2 molecules for both the two systems.