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arXiv:1408.1794 · Europhysics Letters (EPL)

All-optical production and trapping of metastable noble-gas atoms down to the single-atom regime

M. C. Kohler, Heiner Daerr, Peter Sahling, Carsten Sieveke, Norman Jerschabek, Martin Kalinowski, C. Becker, K. Sengstock

Published Oct 1, 2014• 13 citations
arXivHTMLPDF

Abstract

The determination of isotope ratios of noble-gas atoms has many applications, e.g. , in physics, nuclear-arms control, and Earth sciences. For several applications, the concentration of specific noble-gas isotopes ( e.g. , Kr and Ar) is so low that single-atom detection is highly desirable for a precise determination of the concentration. As an important step in this direction, we demonstrate the operation of a krypton atom trap trace analysis (ATTA) setup based on a magneto-optical trap (MOT) for metastable Kr atoms excited by all-optical means. Compared to other state-of-the-art techniques for preparing metastable noble-gas atoms, all-optical production is capable of overcoming limitations regarding minimal probe volume and avoiding cross-contamination of the samples. In addition, it allows for a compact and reliable setup. We identify optimal parameters of our experimental setup by employing the most abundant isotope 84 Kr, and demonstrate single-atom detection within a 3D MOT.

DOI
10.1209/0295-5075/108/13001

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The determination of isotope ratios of noble-gas atoms has many applications, e.g. , in physics, nuclear-arms control, and Earth sciences. For several applications, the concentration of specific noble-gas isotopes ( e.g. , Kr and Ar) is so low that single-atom detection is highly desirable for a precise determination of the concentration. As an important step in this direction, we demonstrate the operation of a krypton atom trap trace analysis (ATTA) setup based on a magneto-optical trap (MOT) for metastable Kr atoms excited by all-optical means. Compared to other state-of-the-art techniques for preparing metastable noble-gas atoms, all-optical production is capable of overcoming limitations regarding minimal probe volume and avoiding cross-contamination of the samples. In addition, it allows for a compact and reliable setup. We identify optimal parameters of our experimental setup by employing the most abundant isotope 84 Kr, and demonstrate single-atom detection within a 3D MOT.
Radioisotopes that break down at a constant rate over time through radioactive decay allow scientists to understand the development of geological and anthropological history by dating samples that contain such isotopes. While many techniques exist to measure the age of a sample, in this thesis we explore the possibility of enhancing the atom trap trace analysis (ATTA) method, which has made significant strides in the area of ultra-sensitive radioisotope detection, especially with the use of metastable noble gas radionuclides. A metastable atom is an atom in a stable, long-lived (>1 ms) excited state. Noble gases have the longest metastable lifetimes, which combined with their geochemical inertness, make them ideal candidates for geological and environmental radiometric techniques. The production of metastable noble gases for this purpose has traditionally relied on discharge sources, but this method suffers from important drawbacks such as high levels of crosscontamination and poor excitation efficiencies. In an effort to overcome these drawbacks, the method described in this work presents a new platform for implementing, characterising and comparing purely laser-based production of metastable noble gases. In the first part of this thesis, we present both state-of-the-art experimental results in the purely laser-based generation of metastable krypton atoms, and a physically realistic simulation with good agreement with our experimental results. Our calculation of the twophoton absorption cross section for krypton (to a metastable-generating excited state) using 215nm deep ultraviolet (DUV) laser radiation, obtained by fitting with theory, confirms that high metastable production efficiencies are possible with laser-based techniques. In addition to this parameter, the branching ratio and photoionisation rate from the excited state are calculated and agree with the literature. In the second part, we present the experimental progress to date for a brand new method of manipulating metastable noble gas atoms using a two-stage approach of metastable production then trapping via a magneto-optical trap (MOT). While the results are limited due to experimental difficulties, they are complemented by a physically realistic 3D simulation based on the Monte Carlo method. This simulation suggests that the production and trapping of metastable noble gases is feasible without the use of a discharge source, a Zeeman slower, and even a secondary excitation chamber. However, the loading rate for such a MOT is not sufficient for ATTA measurements without drastic changes in the experimental configuration. In the final part, we propose a next-generation ATTA system based on stimulated rapid adiabatic passage (STIRAP) to transfer noble gas atoms to their metastable state with near 100% efficiency. This technique for the generation of metastable noble gases would be purely laser-based and would compete with the loading rates of conventional production techniques, while avoiding their deleterious effects. We conclude by identifying limits of laser-based techniques and explore approaches to overcome them.
We have demonstrated that the ion current resulting from collisions between metastable krypton atoms in a magneto-optical trap can be used to precisely measure the trap loading rate. We measured both the ion current of the abundant isotope 83Kr (isotopic abundance=11%) and the single-atom counting rate of the rare isotope 85Kr (isotopic abundance∼1×10(-11)), and found the two quantities to be proportional at a precision level of 0.9%. This work results in a significant improvement in using the magneto-optical trap as an analytical tool for noble-gas isotope ratio measurements, and will benefit both atomic physics studies and applications in the earth sciences.
A new method of ultrasensitive trace-isotope analysis has been developed based upon the technique of laser manipulation of neutral atoms. It has been used to count individual {sup 85}Kr and {sup 81}Kr atoms present in a natural krypton sample with isotopic abundances in the range of 10{sup {minus}11} and 10{sup {minus}13}, respectively. The atom counts are free of contamination from other isotopes, elements,or molecules. The method is applicable to other trace-isotopes that can be efficiently captured with a magneto-optical trap, and has a broad range of potential applications.
Laser manipulation of neutral atoms has been used to count individual krypton-85 and krypton-81 atoms present in a natural krypton gas sample with isotopic abundances in the range of 10(-11) and 10(-13), respectively. This method of isotope trace analysis is free of contamination from other isotopes and elements and can be applied to several different isotope tracers for a wide range of applications. The demonstrated detection efficiency is 1 x 10(-7). System improvements could increase the efficiency by many orders of magnitude.
Atom-Trap Trace-Analysis (ATTA) is a technique aimed at a measuring the relative (in comparison to the common isotope) abundance of exceedingly rare noble gas radio-isotopes (Ar-39, Kr-81 and Kr-85), for the purposes of dating water, ice and other materials that contain trapped gases. These isotopes exist with an extremely low natural abundance and require measurement capability down to parts in 1017. The noble gas dating protocol is similar to that of radio-carbon dating but, the three isotopes together, allow dating of materials in complementary ranges to that possible with the radiocarbon technique. In a facility jointly created by CSIRO, Griffith and Adelaide Universities, we use laser guidance, cooling and trapping to perform isotopic separation using the isotopic dependence of atomic energy levels. The facility is currently undergoing construction but has been shown to be able to produce metastable Ne and Ar, which can then be laser cooled and trapped. When combined with the existing gas separation facility at the CSIRO Waite facility, which efficiently extracts pure noble gases from that are dissolved in water or ice samples, we should be in a position to start measuring the age of real-world samples in the early part of 2020. In addition, to describing the current state of construction, we will also discuss two more efficient approaches for creating metastable atoms that can reduce samples size and avoid unwanted cross-contamination between samples.
We have developed an atom trap trace analysis (ATTA) system to measure Kr in Xe at the part per trillion (ppt) level, a prerequisite for the sensitivity achievable with liquid xenon dark matter detectors beyond the current generation. Since Ar and Kr have similar laser cooling wavelengths, the apparatus has been tested with Ar to avoid contamination prior to measuring Xe samples. A radio-frequency plasma discharge generates a beam of metastable atoms which is optically collimated, slowed, and trapped using standard magneto-optical techniques. Based on the measured overall system efficiency of 1.2 × 10(-8) (detection mode), we expect the ATTA system to reach the design goal sensitivity to ppt concentrations of Kr in Xe in <2 h.