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AIP conference proceedings

Towards trace detection of [sup 85]Kr by two-step excitation and field ionization

Xinghua Li

Published Jan 1, 2001• 0 citations
Publisher

Abstract

We have implemented a new laser-based detection scheme for the rare krypton isotopes. The scheme utilizes two-step excitation of metastable krypton atoms in a nearly perfect three-level system followed by field ionization. The detection scheme was realized experimentally with a mass-separated atom beam. A total detection efficiency of about 10% is obtained.

DOI
10.1063/1.1405584

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We have implemented a new laser-based detection scheme for the rare krypton isotopes. The scheme utilizes two-step excitation of metastable krypton atoms in a nearly perfect three-level system followed by field ionization. The detection scheme was realized experimentally with a mass-separated atom beam. A total detection efficiency of about 10% is obtained.
A new method of ultrasensitive isotope trace analysis has been developed. This method, based on the technique of laser manipulation of neutral atoms, has been used to count individual {sup 85}Kr and {sup 81}Kr atoms present in a natural krypton gas sample with isotopic abundances in the range of 10{sup {minus}11} and 10{sup {minus}13}, respectively. This method 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{sup {minus}7}. System improvements could increase the efficiency by many orders of magnitude.
We have investigated a new scheme for excitation of the 5s, J = 2 metastable level of Kr (5s[3/2] J = 2 ) which can be readily extended to other rare gases. In the scheme, an ultraviolet (UV) lamp is used to create a population of Kr atoms in the 5s[3/2] J = 1 level in a gas cell. The excited atoms are then pumped to the 5p[3/2] J = 2 level, using 819 nm light from a Ti:sapphire laser, from which they decay to the metastable state with a branching ratio of 77%. We made two striking observations: (1) the laser power required to saturate the second step decreases markedly as a function of gas cell pressure, and (2) the UV photon flux is converted with very high efficiency (≈10%) to metastable atom flux. A Monte Carlo study of the scattering of UV photons in the cell reproduces the trends observed. The understanding achieved points to the design of a higher flux source of metastable atoms.
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.
We have devised a simple new scheme to increase the isotopic selectivity in optical rare-isotope detection experiments. We can effectively remove interfering isotopes from an atomic beam by optically pumping them into a state that is invisible to the optical detection system. The selectivity of this resonant depletion scales exponentially with the isotope shift and yields almost unlimited selectivity in principle. We have demonstrated a selectivity of 2.3 x 10(5) with a single laser excitation in a beam of metastable krypton atoms. With better laser stability we may be able to improve the selectivity much further.
A room-temperature beam of krypton atoms in the metastable 5s[3/2]2 level is demonstrated via an optical excitation method. A Kr-discharge lamp is used to produce vacuum ultraviolet photons at 124 nm for the first-step excitation from the ground level 4p6 1S0 to the 5s[3/2]1 level. An 819 nm Ti:sapphire laser is used for the second-step excitation from 5s[3/2]1 to 5s[3/2]2 followed by a spontaneous decay to the 5s[3/2]2 metastable level. A metastable atomic beam with an angular flux density of 3 x 10(14) s(-1) sr(-1) is achieved at the total gas flow rate of 0.01 cm3/s at STP (or 3 x 10(17) at./s). The dependences of the flux on the gas flow rate, laser power, and lamp parameters are investigated.
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.