High-resolution diode-laser spectroscopy on a fast beam of metastable atoms for detecting very rare krypton isotopes

A fast krypton ion beam with an energy of 10 keV is transferred through a mass filter and neutralized in a Rb- (or Cs-) vapour charge exchange cell. The emerging beam of metastable Kr atoms of a selected Kr isotope is collinearly irradiated with a tunable cw GaAlAs diode laser at 811 nm. The spectrum of the 1s ₅–2p ₉ transition covers 10 GHz and consists of one line each for the five stable isotopes of Kr with even mass number and 15 hyperfine structure lines of⁸³Kr. The individual lines are recorded by detecting the fluorescence signal perpendicular to the beams. Photons are guided to the PM tube by diffuse reflection from a high reflectance thermoplastics light collector. Up to 20 photons per atom are emitted by cycling between the two states during the flight time of 1.2 µs through the detector. The observed absorption linewidth of 100 MHz is a combination of laser linewidth and energy uncertainty in the fast atomic beam. In order to achieve maximum isotope selectivity the beam energy has to be adjusted in such a way that the Doppler shifted lines of all isotopes form an optimum pattern for detecting the very rare isotopes⁸¹Kr and⁸⁵Kr in natural environmental samples.     

Laser photoionization detection of the rare isotope3He

Based on combination of the two-step collinear isotope-selective photoionization and time-of-flight separation of atoms in a fast modulated beam, a new technique has been developed for detecting the³He rare isotope with an isotopic selectivity of up to 10¹⁰. The technique helped to detect optically, for the first time,³He at a relative abundance of 4·10^–8.     

Hyperfine structure induced isotopic effects in krypton resonance ionization mass spectrometry

A time-of-flight mass spectrometer combined with a pulsed laser system has been used for determination of krypton isotope ratios of air samples containing 10⁶-10⁷ krypton atoms. A three-color, doubly resonant ionization scheme employing a 116.48 nm transition from the ground into the first 4s²4p⁵(²P°_1/2)5s J = 1 excitation level has been applied. The magnitude of a hyperfine splitting of this level has been estimated for ⁸¹Kr, ⁸³Kr and ⁸⁵Kr isotopes. Hyperfine structure induced isotopic effects have been investigated under different saturation conditions and found to be negligible when the first and the second transitions are strongly saturated.     

Continuous wave field ionization laser spectroscopy

A new technique is described which allows Doppler-free, isotope-selective excitation of atoms by continuous wave laser radiation and continuous ionization of the atoms by an electric field. The atoms are excited to high Rydberg states in an electric-field-free region of a collimated atomic beam. Because the lifetimes of Rydberg atoms are long they can reach a spatially separated region of the atomic beam where they are ionized by a continuous electric field with a probability of unity. In the case of lithium we obtained a 10³ times larger ion signal by field ionization of Rydberg atoms than by direct photoionization from low excited states.     

Laser resonant ionization of plutonium

Resonance ionization mass spectrometry (RIMS) has been tested for the isotope-selective determination of trace amounts of plutonium. An atomic beam is formed by evaporating plutonium atoms from a rhenium-filament heated to 1800 °C. The radiation of a pulsed dye laser excites the atoms in a two-photon process (=595.2 nm) followed by photoionization of the excited atoms. Mass selectivity is obtained by use of a time-of-flight spectrometer. A resonant signal of²³⁹Pu was measured with 10¹³ atoms deposited on the filament.     

Atom trap trace analysis

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 ⁸⁵Kr and ⁸¹Kr atoms present in a natural krypton gas sample with isotopic abundances in the range of 10⁻¹¹ and 10⁻¹³, respectively. The method is free of contamination from other isotopes and elements, and can be applied to many different isotope tracers for a wide range of applications. This revised version was published online in August 2006 with corrections to the Cover Date.     

Reliability evaluation for failed fuel identification using resonance ionization mass spectrometry

In the fast reactors, rapid and accurate identification of a fuel failure event is essential for ensuring safety operation. Isotopic analysis of krypton (Kr) and xenon (Xe) using resonance ionization mass spectrometry (RIMS) is an effective identification tool, in which Kr and Xe atoms are resonantly ionized by a pulsed laser at 216.7 nm and 249.6 nm, respectively, and then three isotopic ratios: ⁷⁸Kr/⁸⁰Kr, ⁸²Kr/⁸⁰Kr and ¹²⁶Xe/¹²⁹Xe are measured to detect the location of the failed fuel assembly. In this paper, we report on the required analytical precision of RIMS estimated from simulation studies as well as the analytical performance of our spectrometer to evaluate the availability of RIMS to the failed fuel identification technique in the fast reactors.     

用激光计数放射性氪原子

原子阱痕量分析是一种基于激光的新方法,能够对数微升氪气中丰度低至10^-14的⁸⁵Kr和⁸¹Kr原子进行计数测量．介绍了在合肥建成的痕量放射性氪同位素测量系统,包括ATTA装置、水中溶解气提取和氪气分离提纯的样品处理设备．利用该系统对国内多处大气中⁸⁵Kr浓度的测量结果为1.3～1.6 Bq/m³,与文献中北半球大气本底值相吻合．对华南和华北的几个浅层和深层地下水样品进行了⁸⁵Kr和⁸¹Kr测年,示范了该系统的应用．     

异核双原子和三原子分子在红外强激光场中的电离抑制

Ionization is the fundamental process in interaction of atoms/molecules with femtosecond strong laser fields. Comparing to atoms, molecules exhibit peculiar behaviors in strong-field ionization because of their diverse geometric structures, molecular electronic orbitals as well as extra nuclear degrees of freedom. In this study, we investigate strong field single and double ionization of carbon monoxide (CO) and carbon dioxide (CO₂) in linearly polarized 50-fs, 800-nm laser fields with peak intensity in the range of 2×10¹³ W/cm² to 2×10¹⁴ W/cm² using time-of-flight mass spectrometer. By comparing the ionization yields with that of the companion atom krypton (Kr), which has similar ionization potential to the molecules, we investigate the effect of molecular electronic orbitals on the strong-field ionization. The results show that comparing to Kr, no significant suppression is observed in single ionization of both molecules and in non-sequential double ionization (NSDI) of CO, while the NSDI probability of CO₂ is strongly suppressed. Based on our results and previous studies on homonuclear diatomic molecules (N₂ and O₂), the mechanism of different suppression effect is discussed. It is indicated that the different structure of the highest occupied molecular orbitals of CO and CO₂ leads to distinct behaviors in two-center interference by the electronic wave-packet and angular distributions of the ionized electrons, resulting in different suppression effect in strong-field ionization.     

The excited states of Kr and Rb isotopes in the 78 ≦ A ≦ 85 mass region

The excited states of the ^{78, 80, 81}Kr and ^{80, 81, 83}Rb nuclei were investigated in radio-active decays of the respective Rb and Sr isotopes. The level schemes were established and for a number of levels the spin-parity assignments suggested on the basis of the log ft values and γ-branching ratios, as well as in some cases angular-correlation results. The structures of excited states of the odd Kr, odd Rb, and doubly even Kr isotopes are compared and discussed in the framework of existing theoretical approaches.     

Collisional relaxation of ionic2 P 3/2 excited states in rare gases

Optical pumping with theD ₂ line is used to study the depolarization of the first excited² P _3/2 states of alkaline earth ions and Yb⁺ ions in collisions with rare gas atoms. The deorientation cross sections for the even isotopes of Ba⁺ and Yb⁺ ions are obtained (in units of 10^?16 cm²): rare gas He Ne Ar Kr Xeσ ₁ (Ba⁺ 6p ² P _3/2) 79(11) 89(13) 123(18) 152(22) 204(30)σ ₁ (Yb⁺ 6p ² P _3/2) 60(10) 62(9) 107(18) 133(17) 167(37) The cross sections are discussed in comparison with theoretical calculations and those of isoelectronic atoms. The comparison of the² P _3/2 relaxation of even and odd (I=3/2) isotopes of Ba⁺ allows to draw conclusions on the nature of the depolarization interaction.     

Laser Based Techniques for Ultra Trace Isotope Production, Spectroscopy and Detection

A variety of research activities in the field of fundamental and applied nuclear physics has evolved in the last years using resonantly tuned radiation from powerful lasers. The technique of resonance ionization spectroscopy has delivered outstanding results and found broad acceptance in the last years as a particularly efficient and highly selective method for rare and exotic radioisotope studies. It is used for production, spectroscopy and detection of these species and provides complete isobaric, high isotopic and even some isomeric selection, which altogether is needed for on-line investigation of short lived species far off stability as well as for ultra trace determination. Good overall efficiency pushes the experimental limits of detection in elemental trace analysis down to below 10⁶ atoms per sample, and additionally isotopic selectivity as high as 3 × 10¹² has been demonstrated. The widespread potential of resonance ionization techniques is discussed, focusing on the experimental arrangements for applications in selective on-line isotope production, spectroscopy of rare radioisotopes and ultra trace determination of radiotoxic isotopes like ²³⁸Pu to ²⁴⁴Pu, ^135,137Cs, ^89,90Sr or ⁴¹Ca in environmental, technical and biomedical samples.     

Rotational spectra of the Kr-H2O van der Waals complex

Rotational spectra of the Kr-H₂O van der Waals complex were measured in the frequency range 4–19 GHz using a pulsed jet cavity Fourier transform microwave spectrometer. The isotopomers studied include those of H₂O, HDO, D₂O, H₂ ¹⁷O and H₂ ¹⁸O with the six most abundant isotopes of Kr. A tunnelling splitting due to a large amplitude internal motion of the H₂O subunit that exchanges bonded and non-bonded hydrogen atoms was observed. Nuclear quadrupole hyperfine structure was resolved and measured for the complexes containing ⁸³Kr, D, and ^l7O, and the corresponding nuclear quadrupole coupling constants were determined. These were used to estimate structural parameters and to derive information about the intermolecular dynamics. The results, and in some instances the spectroscopic constants themselves, were compared with experimental and theoretical data previously reported for Ar-H₂O.     

Measurement of the rate of nuclear capture of negative muons in the isotopes 84Kr and 136Xe

The lifetime of a negative muon in the 1S state in the isotopes ⁸⁴Kr and ¹³⁶Xe was measured. The values obtained, τ(⁸⁴Kr)=139.2±2.9 ns and τ(¹³⁶Xe)=111.0±4.6 ns, correspond to total nuclear capture rates Λ_c(⁸⁴Kr)=6.75±0.15 μs⁻¹ and Λ _c(¹³⁶Xe)=8.6±0.4 μs⁻¹. Theoretical calculations of the rate of nuclear capture of a negative muon are performed for the Kr isotopes. The experimental results are compared with the theoretical calculations. Pis’ma Zh. éksp. Teor. Fiz. 67, No. 5, 302–307 (10 March 1998)     

Streuung von Li+-Ionen an Edelgasen

The angular distribution of Li ₇ ⁺ -ions (7–60 keV) scattered by rare gas atoms (He, Ne, A, Kr, X) shows 3–5 characteristic maxima of intensity, which are not observed when electrons of equal energy are scattered by the same atoms. The existence of the maxima can be explained by polarization of the scattering rare gas atoms by the Li ₇ ⁺ -ions.     

Laser method of highly selective detection of rare radioactive isotopes through multistep photoionization of accelerated atoms

A laser detection method is proposed for ultralow abundance (<10^–10) of rare radioactive isotopes based on a multistep photoionization of accelerated atoms with a selectivity up to 10⁷ on each step of a collinear laser excitation.     

Optical pumping of ions in buffer gases

Transient signals measured with a pulsed rf-optical pumping method are used to determine longitudinal relaxation rates for Sr⁺ ions (even isotopes) in noble gas buffers. Depolarization cross sections of the electronic spin in the Sr⁺5² S _1/2 ground state for binary collisions with rare gas atoms are deduced. The results for σ(Sr⁺5² S _1/2) in Ų are (at temperatures between 374 and 449 °K): 2·10^?5(He),4·10^?5(Ne), 5.7·10^?3(Ar), 1.8·10^?2(Kr), and 4.0·10^?2(Xe). These cross sections for the Sr⁺ ion are about two to three orders of magnitude larger than the corresponding ones for the isoelectronic neutral Rb atom. The large increase of the Sr⁺ relaxation rates is explained with the relaxation mechanism of spin-orbit coupling, taking into account two “indirect” effects of the ionic charge: the increase in the gas kinetic cross sections and the more intimate collisions of the Sr⁺ ion with the noble gas atoms. The depolarization is shown to be predominantly due to short-range interactions. A contribution to the relaxation of the Sr⁺ ion from Sr⁺-noble gas molecule formation, induced by three-body or resonant two-body collisions, could not be established for applied pressuresp between 1.5 and 15 Torr of Ar, Kr, and Xe.     

Independent yields of Kr and Xe isotopes in the photofission of heavy nuclei

The yields of Kr (A = 87–93) and Xe (A = 138–143) primary fission fragments produced in ²³²Th, ²³⁸U, and ²⁴⁴Pu photofission upon the scission of a target nucleus and neutron emission were measured in an experiment with bremsstrahlung from electrons accelerated to 25 MeV by a microtron, and the results of these measurements are presented. The experimental procedure used involved the transportation of fragments that escaped from the target by a gas flow through a capillary and the condensation of Kr and Xe inert gases in a cryostat at liquid-nitrogen temperature. The fragments of all other elements were retained with a filter at the capillary inlet. The isotopes of Kr and Xe were identified by the γ spectra of their daughter products. The mass-number distributions of the independent yields of Kr and Xe isotopes are obtained and compared with similar data on fission induced by thermal and fast neutrons; the shifts of the fragment charges with respect to the undistorted charge distribution are determined. Prospects for using photofission fragments in studying the structure of highly neutron-rich nuclei are discussed.     

Development of accelerator mass spectrometry assisted by isotope-selective laser photodetachment for monitoring 129I

A prototype system was developed to investigate an isotope-selective laser photodetachment technique for a ¹²⁹I accelerator mass spectrometer. A pulsed ion source for negative iodine ions (I⁻) that employed laser ablation proved to be suitable for isotope-selective laser photodetachment. Laser photodetachment of pulsed negative iodine ions was estimated to have an efficiency of about 81% based on a model calculation for the prototype system with a tunable pulsed Ti:sapphire laser.     

A study of the VUV emission from highly ionized krypton in a theta pinch plasma

The ionization rates of Kr(IX), (X), (XI), and (XII) have been measured using a fast 60-kV-60kJ theta pinch as a plasma source. The line emission from each ion stage has been identified and the time evolution observed. A coupled set of rate equations was used along with time- and space-resolved measurements of the electron density and temperature to model the plasma light emission. The ionization rates of Kunze were adjusted by multiplying the rate for each ion stage with a constant until the peak intensity of the calculated emission agreed with the time of the observed peak intensity. The constants required for best fit were 2.5, 0.15, 3.0, and 2.0 for Kr(IX), (X), (XI), and (XII), respectively. Two successive ionization stages, Kr(X) and Kr(XI), have shown the same time dependence and possible reasons for this observation are discussed. During the course of modeling the light emission, we have also found that the rate for the excitation from the 3dⁿ to the 3p⁵3dⁿ⁺¹ level in Kr(X) (n=9) and Kr(XI) (n=8) is a factor of 5 lower than predicted by the van Regemorter excitation rate equation.