Detection of very rare isotopes by laser collinear resonant ionization of fast atoms

Results are presented of the work on the development of a method for detecting ultra rare isotopes, based on the collinear isotope-selective laser ionization of atoms in a fast bearn. The rare isotope³He was detected at a selectivity of 10⁹ and isotope-selective ionization of krypton atoms was demonstrated. A scheme is suggested for detecting the rare radioactive isotopes⁸⁵Kr and⁸¹Kr. The technique has been exploited for the measurement of hyperfine structures and isotope shifts of unstable Yb isotopes.     

Resonance Ionization Mass Spectrometry (RIMS) with Pulsed and CW-Lasers on Plutonium

The detection of long-lived plutonium isotopes in ultra-trace amounts by resonance ionization mass spectrometry (RIMS) is a well-established routine method. Detection limits of 10⁶ to 10⁷ atoms and precise measurements of the isotopic composition have been achieved. In this work multi-step resonance ionization of plutonium atoms has been performed with tunable lasers having very different output intensities and spectral properties. In order to compare different ways for the resonance ionization of plutonium broadband pulsed dye and titanium:sapphire lasers as well as narrow-band cw-diode and titanium:sapphire lasers have been applied for a number of efficient excitation schemes. It has been shown, that for identical excitation schemes the optical isotope selectivity can be improved by using cw-lasers (bandwidths < 10 MHz) instead of pulsed lasers (bandwidths > 2 GHz). Pulsed and cw-laser systems have been used simultaneously for resonance ionization enabling direct comparisons of pulsed and continuous ionization processes. So far, a three-step, three-color laser excitation scheme has been proven to be most practical in terms of efficiency, selectivity and laser wavelengths. Alternatively a newly discovered three-step, two-color excitation scheme which includes a strong two-photon transition from an excited state into a high-lying autoionizing state yields similar ionization efficiencies. This two-photon transition was characterized with respect to saturation behavior and line width.     

Loading rate of Yb<Superscript>+</Superscript> loaded through photoionization in radiofrequency ion trap

We investigate the loading rate of Yb⁺ ions loaded through photoionization in a radiofrequency trap. The absolute or relative number of the loaded trapped ions is measured by use of an electric resonance of the secular motion. This method is applicable even in the presence of anharmonicity. In two-color photoionization, where the first-excitation laser drives the ¹S₀–¹P₁ transition in the Yb atom and the second one ionizes the atom from the ¹P₁ state, the loading rate is at its highest by the excitation of the ionization potential. A similar loading rate is observed at the second-laser wavelength around 369.5 nm, which is the wavelength for the cooling transition of Yb⁺. We estimate the loading cross section to be 40(15) Mb for the two-color excitation of the ionization potential. The excitation of the Yb atoms in the Rydberg states is detected by the enhancement of the loading rate. By irradiation with only the first-excitation laser, Yb⁺ is produced at a rate three orders of magnitude smaller than that when the non-resonant two-photon absorption from the ¹P₁ state is the dominant process. We also measure the charge-exchange rate between Yb⁺ and Yb, and discuss its effect on isotope-selective photoionization loading.     

Narrow 3-photon autoionizing resonances in Tl and Yb

Narrow autoionizing resonances have been observed in Yb and Tl using direct 3-photon excitation of ground state atoms. The linewidth is 0.9 cm^-1 in Yb and 0.4 cm^-1 in Tl. Autoionizing levels in both atoms correspond to doubly excited electronic states. This is the first observation of such states in Tl.     

Trace detection of plutonium by three-step photoionization with a laser system pumped by a copper vapor laser

Laser photoionization has been used to detect trace amounts of plutonium. A high sensitivity and selectivity has been achieved by applying three-step excitation and ionization of the plutonium atoms with high pulse-repetition rates and additional mass determination by time-of-flight measurements. A laser system was developed which consists of a copper vapor laser pumping three dye lasers simultaneously. Samples containing between 10¹⁰ and 10¹² atoms of²³⁹Pu on Re filaments were measured yielding strong resonance signals with maximum ion count rates of several kHz at a vanishingly low background. A detection efficiency of 10^–7 was determined allowing the detection of about 10⁸ plutonium atoms in a sample.This work comprises part of the doctoral dissertation of W. Ruster, to be submitted to Johannes-Gutenberg-Universität, Mainz     

Evaluation of Limiting Characteristics of Laser Separation of Silicon Isotopes

Isotopically selective photoionization of silicon atoms by laser radiation using tunable dye lasers is considered. The scheme of atomic ionization with two-photon excitation via the resonance level of one of the high states with subsequent excitation of the autoionization state is proposed. The calculations carried out show that the up-to-date development of laser facilities allows one to evaluate the ultimate production of the highly enriched ²⁸Si isotope at a level of 0.1 g/h at a radiating power of 1 W for each wavelength. The excitation selectivity appears to be high (about 100) within the framework of the radiation problem and is actually defined by the conditions of ion extraction, background atom concentration, charge exchange, and so on rather than by the radiation processes.     

A study of isotopically selective photoionization of ytterbium atoms for laser isotope separation

Atomic-vapor laser isotope separation (AVLIS) is studied experimentally and theoretically for ytterbium vapors. The optimum ionization scheme and the process dynamics are determined. The photoionization scheme uses the transitions $$6^1 S_0 \mathop \to \limits^{555.648nm} 6^3 P_1 \mathop \to \limits^{581.067nm} (7/2,3/2)_2 \mathop \to \limits^{582.79nm} (52353cm^{ - 1} ).$$ For a numerical study of photoionization dynamics, the mathematical model of the AVLIS process is used, which is based on the density matrix formalism and Maxwell's equations. Selective photoionization of the¹⁶⁸Yb isotope is simulated numerically. The yield and selectivity of the process are determined. It is shown that the length of the photoionization region is limited because the laser radiation is absorbed by atoms of¹⁷¹Yb and¹⁷³Yb isotopes. The advantage of the laser method over the method using an electromagnetic separator is demonstrated.     

Wavelength dependent Stark compensation in isotope selective Doppler-free two photon ionization

A novel wavelength dependent Stark shift compensation method for isotope selective ionization in Doppler free two-photon spectroscopy is theoretically investigated. In the present paper, certain wavelengths for the ionization step termed as “magic wavelengths” are identified for compensating the Stark shift induced by the excitation laser. The numerical calculations indicate that, ionization efficiencies can be maximized by the judicious choice of the intensities of the excitation and the ionization lasers without much degradation in the optical selectivity. The effects of Stark shift induced asymmetry and its reversal by selecting the appropriate magic wavelength for the ionization step for various excitation and ionization laser intensities have been investigated. The wavelength dependent Stark compensation method can be adapted for the isotope selective Doppler free two-photon excitation followed by non-resonant ionization process for any atomic system. In the present work, the theoretical results pertaining to the specific example of ⁴¹Ca has been presented.     

A Clear Atomic Example for the Surface Sensitivity of Penning Ionization: He*(23S) + Yb

Using a crossed-beam apparatus with a double hemispherical electron spectrometer, we have studied the spectrum of electrons released in thermal energy ionizing collisions of metastable He*(2³S) atoms with ground state Yb(4f¹⁴ 6s^{2 1}S₀) atoms, thereby providing the first Penning electron spectrum of an atomic target with 4f-electrons. In contrast to the Hel (58.4 nm) and NeI (73.6/74.4 nm) photoelectron spectra of Yb, which show mainly 4f- and 6s-electron emission in about a 5:1 ratio, the He*(2³S) Penning electron spectrum is dominated by 6s-ionization, accompanied by some correlation-induced 6p-emission (8% Yb⁺(4f¹⁴ 6p ²P) formation) and very little 4f-ionization (?2.5%). This astounding result is attributed to the electron exchange mechanism for He*(2³S) ionization and reflects the poor overlap of the target 4f-electron wavefunction with the 1s-hole of He*(2³S), as discussed on the basis of Dirac-Fock wave functions for the Yb orbitals and through calculations of the partial ionization cross sections involving semiempirical complex potentials. The presented case may be regarded as the clearest atomic example for the surface sensitivity of He*(2³S) Penning ionization observed so far.     

Positron scattering and ionization of neon atoms—theoretical investigations

Although positron scattering with inert gas atoms has been studied in theory as well as in experiment, there are discrepancies. The present work reports all the major total cross sections of e+-neon scattering at incident energies above ionization threshold, originating from a complex potential formalism. Elastic and cumulative inelastic scatterings are treated in the complex spherical e+-atom potential. Our total inelastic cross section includes positronium formation together with ionization and excitation channels in Ne. Because of the Ps formation channel it is difficult to separate out ionization cross sections from the total inelastic cross sections. An approximate method similar to electron-atom scattering has been applied to bifurcate ionization and cumulative excitation cross sections at energies from threshold to 2000 eV. Comparisons of present results with available data are made. An important outcome of this work is the relative contribution of different scattering processes, which we have shown by a bar-chart at the ionization peak.     

Laser-induced breakdown of krypton near five-photon ionization threshold

Selective excitation of laser-induced breakdown in krypton in the pressure range 1–4 bar and the spectral range 420–620 nm at a laser intensity of 10¹¹ W/cm² has been studied. It is shown that the breakdown of krypton can be induced selectively due to resonantly enhanced multiphoton ionization via excited atomic states. A number of four- and five-photon atomic resonances have been identified in breakdown excitation spectra. The role of different factors determining the selectivity of the breakdown has been studied. Possible analytical applications of a selective breakdown are discussed.     

The ISOLDE laser ion source for exotic nuclei

At the ISOLDE on line mass separator a system of copper vapor lasers and dye lasers serves for resonant ionization of atoms inside a hot cavity attached to the target. Radioactive ion beams of Yb, Ag, Mn, Ni, Zn, Be, Cu, Cd and Sn were produced with the Resonance Ionization Laser Ion Source (RILIS). Two and three step excitation schemes are used, providing an ionization efficiency of about 10%. Thanks to the use of the RILIS it became possible to ionize beryllium efficiently at ISOLDE, and all particle stable Be isotopes could be separated for the first time. Separation of Ag and Cu nuclear isomers was achieved in the ion source by appropriate tuning of the laser wavelength. New isotopes of Ag, Mn, Zn, Cd and Sn were found, including the r process “waiting point” nucleus ¹²⁹Ag. This revised version was published online in August 2006 with corrections to the Cover Date.     

Quantum-degenerate gases of Ytterbium atoms

Evaporative cooling of ultracold Yb atoms near the quantum-degenerate regime was experimentally studied. Three bosons of ¹⁷⁰Yb, ¹⁷²Yb, ¹⁷⁶Yb and two fermions of ¹⁷¹Yb and ¹⁷³Yb were evaporatively cooled in a crossed far-off resonant trap (FORT). We observed that ¹⁷⁰Yb and ¹⁷²Yb were not concentrated into the crossed region. We found that, in the cases of ¹⁷⁶Yb atoms, atoms were concentrated well into the crossed region. The following evaporative cooling in the crossed region, however, did not work well. We performed the simultaneous trapping and sympathetic cooling in the crossed FORT by use of ¹⁷²Yb-174Yb, ¹⁷⁴Yb-¹⁷⁶Yb, ¹⁷²Yb-¹⁷⁶Yb, and ¹⁷¹Yb-¹⁷⁴Yb pairs. We observed that evaporative cooling worked well. This result shows that we succeeded in the enhancement of the atom collision rate. Especially, by use of ¹⁷⁴Yb-¹⁷⁶Yb mixture, we obtained cold ¹⁷⁶Yb whose phase space density was 0.02. We observed a large atom loss, which limited the further sympathetic evaporative cooling. We also evaporatively cooled ¹⁷⁴Yb in a 1D optical lattice. Evaporative cooling worked very well because the atoms were initially trapped at a high density. After evaporative cooling, we obtained very cold atoms, and T/T _F was estimated to be 1.2.     

Quantum interference effects in field ionization: Application to the measurement of the fine structure splitting of highly excited Na2 D states

Quantum beats between the fine structure levels of highly excitedn ² D levels of sodium atoms have been measured by investigating the field electrons. The states were populated by stepwise excitation with two dye lasers and an electric field pulse was applied a certain time after the laser excitation. The quantum beat signal is observed when the time delay between excitation and ionization is varied. The fine structure splitting forn=21 to 31 has been measured.     

Quadrupole oscillations in a quantum degenerate Bose–Fermi mixture

We study the collective dynamics in a degenerate Bose–Fermi mixture of ¹⁷⁴Yb and ¹⁷³Yb atoms. We excite collective oscillations by a sudden reduction of the trapping confinement and observe low m=0 quadrupole oscillations of condensates in ¹⁷⁴Yb. First the oscillations in ¹⁷⁴Yb atoms alone are investigated, and they are well described by the time-dependent Gross–Pitaevskii equation in the Thomas–Fermi approximation. Using the same procedure the quadrupole oscillations are excited for a ¹⁷⁴Yb–¹⁷³Yb Bose–Fermi mixture. In comparing data taken with and without fermionic ¹⁷³Yb atoms, the oscillation frequency of the quadrupole mode in the condensate decreases with the presence of ¹⁷³Yb atoms.     

The influence of non-radiative transitions on bombardment induced photon emission from Ti and Ti oxide

Photon yields from Ti atoms sputtered from Ti and Ti oxide due to 55 keV Ar⁺ and O₂⁺ ion bombardment have been studied. Photon yields and line profiles of selected lines have also been studied as a function of background O₂ exposure. An attempt has been made to correlate changes in yields and line shapes with variations of the band structure in the solid. Resonance ionization processes are shown not to contribute to the observed yield, however Auger processes cannot be excluded. Lifetime effects have a strong influence on the observed results. It is shown that the distribution of excited states produced by the ion bombardment is Boltzmannlike. We note that it is possible to interpret these results in terms of a model which assumes that the probability of excitation or ionization is exponentially dependent on the excitation or ionization energy, without invoking electron exchange mechanisms.     

Blue up-conversion with excitation into Tm ions at 808 nm in YVO4 crystals co-doped with thulium and ytterbium

The up-conversion of infrared radiation at 808 nm, emitted by a diode laser, into blue emission centered at 480 nm in 1 at.% Tm, 5 at.% Yb: YVO₄; 1 at.% Tm, 8 at.% Yb: YVO₄ and 2 at.% Tm, 5 at.% Yb: YVO₄ has been studied. The highest intensity of blue emission is found for the 1 at.% Tm, 8 at.%Yb: YVO₄ system. The power dependence of up-converted emission upon continuous-wave excitation as well as the time evolution of its intensity upon short-pulse excitation were found to be consistent with a two-step excitation mechanism in which the forward Tm³⁺–Yb³⁺ energy transfer is followed by the back Yb³⁺–Tm³⁺ energy transfer. The effect of dopant concentrations on the up-conversion process is interpreted taking into account dynamics of the excited states involved.     

Resonance ionization mass spectroscopy for trace analysis of neptunium

Resonance ionization mass spectroscopic (RIMS) measurements for trace analysis and spectroscopy of ²³⁷Np, the ecologically most important isotope of neptunium, are described. The chemical procedure for the separation of neptunium from aqueous samples as well as the preparation of filaments for RIMS are outlined. Several two- and three-step excitation schemes have been investigated in order to find suitable conditions for the sensitive detection of ²³⁷Np. Using a three-step, three-color excitation and ionization scheme an overall detection efficiency of 3×10^–8 was obtained, resulting in a detection limit of 4×10⁸ atoms (160 fg) of ²³⁷Np. The hyperfine structure splittings of the levels under investigation, which influence the detection limit, were measured. A new method to determine the first ionization potential (IP) was applied to neptunium yielding a value of IP=6.2655(2) eV.     

On the interaction of an electron with a nonspherical atom

A three-stage scheme for the excitation of the autoionization state of europium atoms is realized, and the corresponding ionization cross section is determined: σ=6.5×10^?10 cm². Analytical signals from europium atoms are recorded in standard and waste water solutions used in mining noble metals and in the diagnostics of rare-earth elements.     

The lattice location and hyperfine field of implanted Yb in Fe as a function of annealing temperature

A combined study has been made of the lattice location and hyperfine field of Yb implanted into Fe single crystals. The location has been determined by ion channeling and back-scattering, the hyperfine field by perturbed angular correlation (PAC) measurements on¹⁶⁹Yb (decaying to excited states in¹⁶⁹Tm). The channeling experiments indicate that initially about 60% of the Yb atoms occupy substitutional sites in the Fe lattice, while the remaining atoms are not in any specific crystallographic site. On annealing, Yb migrates from substitutional to non-substitutional sites. No Yb atoms remain substitutional after a 600°C anneal. By making PAC measurements at two temperatures for two - cascades in¹⁶⁹Tm, it is found that the PAC pattern can be described using a combined static and time-dependent magnetic interaction. The PAC results show that the average hyperfine field and relaxation parameter decrease on annealing, and that the field disappears after a 600°C anneal. The correlation between the location and the hyperfine field is discussed. A comparison of the results with previous Mössbauer results for¹⁵¹Gd implanted in Fe, together with relaxation parameter measurements on a¹⁶⁹Yb₂O₃ source, suggests that the non-substitutional Yb is internally oxidized in the Fe host.Work partly carried out while at the Clarendon Laboratory, Oxford, England and Nuclear Physics Division, AERE, Harwell, England.