Multi-step Resonance Ionization Research Articles

High efficiency resonance ionization of thorium

Multi-step resonance ionization spectroscopy of thorium has been performed with Ti:Sapphire lasers and a hot-cavity laser ion source. Resonance ionization schemes involving three-color, three-photon ionization processes are evaluated and a new three-photon scheme is demonstrated with measured overall ionization efficiency of 38.6(5)%. This high efficiency makes it possible to determine the thorium impurities in materials used for ultra-low background neutrino detectors and could also benefit ultra-trace thorium analysis using resonance ionization mass spectrometry for various radiochemical tracer applications.

Resonant ionization spectroscopy of autoionizing Rydberg states in cobalt and redetermination of its ionization potential**This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to

Multi-step resonance ionization spectroscopy of cobalt has been performed using a hot-cavity laser ion source and three Ti:Sapphire lasers. The photoionization spectra revealed members of five new autoionizing Rydberg series that originate from three different lower levels of 3d74s5s h4F9/2, 3d74s4d f4G11/2, and 3d74s4d f4H13/2 and converge to the first four excited states of singly ionized Co. The analyses of the Rydberg series yield 63 564.689 ± 0.036 cm−1 as the first ionization potential of Co, which is an order of magnitude more accurate than the previous estimation. Using a three-step resonance ionization scheme that employs an autoinizing Rydberg state in the last transition, we obtained an overall ionization efficiency of about 18% for Co.

Control of RILIS lasers at IGISOL facilities using a compact atomic beam reference cell

The choice and proper operation of the laser systems for laser ion sources at on-line facilities using multi-step resonance ionization processes is the basis for production of intense and pure radioactive ion beams. These pave the way for numerous fundamental studies in nuclear and astrophysics. A comparison between systems of medium or high repetition rate pulsed tunable lasers based on dyes or crystals as active medium has been carried out at the IGISOL facility at Louvain-la-Neuve. The importance of properly controlling the operation conditions of the individual lasers via a reference atomic beam chamber is highlighted and design and implementation of such a compact device for permanent monitoring as well as possible regulation of the various laser parameters of relevance is discussed.

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 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.

Multi-color resonance ionization of laser ablated gadolinium at high laser power

Spectroscopic and analytical properties of a trace analytical method using multi-step resonance ionization at high laser intensities (>kW/cm2) have been investigated with gadolinium as a test element. Strongly saturated transitions are observed, which have been used for a temperature determination of the atoms in the laser ablated plume. Regimes of multi-step resonance ionization and multiphoton ionization could be distinguished. Analytical performances due to resonance enhancement and resulting discrimination against non-resonant background, precision in isotope ratio determination and overall detection efficiency are discussed.

Trace determination of gadolinium in biomedical samples by diode laser-based multi-step resonance ionization mass spectrometry.

The application of high-resolution multi-step resonance ionization mass spectrometry (RIMS) to the trace determination of the rare earth element gadolinium is described. Utilizing three-step resonant excitation into an autoionizing level, both isobaric and isotopic selectivity of >10(7) were attained. An overall detection efficiency of approximately 10(-7) and an isotope specific detection limit of 1.5 x 10(9) atoms have been demonstrated. When targeting the major isotope (158)Gd, this corresponds to a total Gd detection limit of 1.6 pg. Additionally, linear response has been demonstrated over a dynamic range of six orders of magnitude. The method has been used to determine the Gd content in various normal and tumor tissue samples, taken from a laboratory mouse shortly after injection of gadolinium diethylenetriaminepentaacetic acid dimeglumine (Gd-DTPA), which is used as a contrast agent for magnetic resonance imaging (MRI). The RIMS results show Gd concentrations that vary by more than two orders of magnitude (0.07-11.5 microg mL(-1)) depending on the tissue type. This variability is similar to that observed in MRI scans that depict Gd-DTPA content in the mouse prior to dissection, and illustrates the potential for quantitative trace analysis in microsamples of biomedical materials.

Investigation of Rydberg states of the europium atomusing resonance ionization spectroscopy

We report four odd-parity Rydberg series in the spectrum ofeuropium atoms in the energy region 45 000-45 735 cm-1.These four series belong to total angular momentum quantumnumbers J = 5/2,7/2,9/2 and 11/2 and converge to the firstionization limit 9S4. The studies were carried outemploying the multistep resonance ionization spectroscopytechnique using two pulsed dye lasers. For some of the Rydbergseries we could observe the members up to n = 67. Differentstepwise excitation-ionization schemes helped us to assign aunique J quantum number up to n = 39 and enabled us to separatethe series with different values of J. The Rydberg seriesbelonging to J = 5/2 was found to be quite unperturbed and wastherefore used to evaluate the first ionization limit of theeuropium atom.

Line shapes in triple-resonance ionization spectroscopy

Line shapes in high-resolution triple-resonance ionization spectroscopy have been calculated and compared with experimental measurements on the 4s2 1S0 --> 4s4p 1P1 --> 4s4d 1D2 --> 4snf 1F3 --> Ca+ system of calcium. Calculations based on the density matrix formalism integrated the fundamental equations over experimental atomic angular and velocity distributions and laser intensity profiles. The measurements reveal and confirm all predicted structures arising from the complex coupling of four atomic states with three laser fields and the Doppler distribution of the atomic ensemble. Effects of different laser beam geometries on the line shapes have been investigated. The agreement between calculated and experimental spectra is generally good over a dynamic range of 10 orders of magnitude. Thus these calculations can accurately predict optical isotopic selectivity in multistep resonance ionization, with a value of S(opt) approximately 10(10) expected for detection of the ultratrace isotope 41Ca.

Selective ultratrace analysis of 41 Ca by laser resonance ionization

A compact resonance ionization mass spectrometer is presented. It is presently applied for sensitive and highly selective ultratrace determination of the long-lived radioisotope 41Ca for environmental, biological, and fundamental investigations. The development of coherent multistep resonance ionization enables the realization of experimental detection limits as low as106 atoms per sample and very high isotopic selectivity above 1012.

Determination of the Pu autoionizing level angular momenta by a multistep excitation with linearly polarized laser light

The modified polarization spectroscopy method was applied for determination of angular momenta of autoionizing states of Pu in multistep resonance ionization processes. In comparison with the known one, our method does not require circular polarization at all, only linear polarizations are needed. This simplicity was reached using a three-dimensional excitation geometry. Angular momenta of nine new autoionizing 242Pu states were determined. The method suggested could be applied for efficiency improvement in multistep RIMS applications as well as for the odd-even isotope separation for elements with a J=0 ground state (Pu, Yb, Sm etc.).

A new experimental method in the study of ionic Rydberg states by resonance ionization mass spectroscopy

We report a new method for detecting highly excited ions. With a strong constant electric field ionization following the extracting of ions by a pulsed electric field in a time-of-flight mass spectrometer, the direct multi-photon ionization background can be eliminated in laser multi-step resonance ionization mass spectroscopy of ionic Rydberg states. A high detection efficiency can be obtained for low members of ionic Rydberg states by use of this method. We have applied the method in the study of the spectroscopy of ionic Rydberg states in ytterbium.

First Determination of the Ionization Potential of Americium and Curium

By multistep resonance ionization with lasers, followed by mass spectrometry, the first ionization potential of neutral atoms can be measured with quantities of only about one nanogram. The ionization potentials of americium (5.9736(3) eV) and of curium (5.9914(2) eV) were thus determined for the first time. The figure on the right shows a plot of the number of ions N versus the total photon energy Etot of three laser beams, which are essential for the experiment. The arrow points to the ionization threshold.

Investigation of lutetium rydberg states by laser multistep resonance ionization spectroscopy

Laser multistep excitation and electric-field ionization spectroscopy have been used to investigate experimentally highly excited states (HES) of lutetium in the vicinity of the first ionization limit. The investigation includes the measurement of energy levels (ionic signal vs last transition frequency) and radiation lifetime (ionic signal vs ionizing electric-field pulse delay) of the states investigated. Even Rydberg states of 4f14 6s2nd have been observed with two-step laser excitation. The maximum experimental error is 0.3 cm−1 for the energy and 20% for the radiation lifetime measurements. This is the very first time that results for the lifetimes as well as for a large part of the energy values have been obtained. Our present experimental results compare well with previously calculated values obtained by relativistic perturbation theory using the zero-order model approximation, and with the available experimental values.

Pulsed single-mode laser ionization of hyperfine levels of zirconium-91

We identify a considerable improvement in proposed schemes for isotopic depletion of zirconium-91 on the basis of the atomic vapor laser isotope separation (AVLIS) method. The improvement lies in applying a single-longitudinal-mode dye laser for selective excitation of all hyperfine split levels of the ground state of zirconium-91. High-resolution laser-induced fluorescence spectroscopy of atomic beams of zirconium produced through laser vaporization–supersonic expansion has been used to identify transitions of zirconium with suitable hyperfine structure. Casimir magnetic-dipole and electric-quadrupole coupling constants and isotope shifts have been derived and are reported for five excited configurations. Suitable intermediate levels in a multistep resonance ionization pathway have been identified by two-color resonance ionization spectroscopy. Isotope depletion has been demonstrated on one ground-state-transition ( z F33∘←a F32at 593.7 nm) by using a specially constructed pulsed, single-longitudinal-mode dye-laser oscillator. Prospects and future directions in zirconium AVLIS are discussed.