Resonance ionization mass spectrometry for precise measurements of isotope ratios

Levine, Jonathan L; Savina, M. R.; Stephan, T.; Dauphas, N.; Davis, A. M.; Knight, Kim B.; Pellin, Michael J.

doi:10.1016/j.ijms.2009.07.013

Cited by 47 publications

(50 citation statements)

References 35 publications

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“…After a short, field-free duration, the secondary neutrals are intersected with three, pulsed laser beams at ~1 mm from the sample surface. The lasers are wavelength tunable Ti:sapphire systems that have been described in detail elsewhere [12,13]. The laser wavelengths are tuned to excite two resonance transitions and an autoionizing state to selectively ionize neutral uranium atoms within the sputtered flux.…”

Section: Methodsmentioning

confidence: 99%

RIMS analysis of ion induced fragmentation of molecules sputtered from an enriched U3O8 matrix

Willingham

Savina

Knight

et al. 2012

J Radioanal Nucl Chem

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Section: Methodsmentioning

confidence: 99%

RIMS analysis of ion induced fragmentation of molecules sputtered from an enriched U3O8 matrix

Willingham

Savina

Knight

et al. 2012

J Radioanal Nucl Chem

Self Cite

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“…One of the great advantages of RIMS is that it uses a finely tuned laser beam to selectively ionize the neutral atoms of a given element sputtered from the sample by an ion beam or desorbed by a laser pulse (43,44). These ions are then analyzed for their masses in a time of flight (TOF) mass spectrometer.…”

Section: Rimsmentioning

confidence: 99%

Laboratory technology and cosmochemistry

Zinner¹,

Moynier²,

Stroud

2011

Proc. Natl. Acad. Sci. U.S.A.

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Recent developments in analytical instrumentation have led to revolutionary discoveries in cosmochemistry. Instrumental advances have been made along two lines: ( i ) increase in spatial resolution and sensitivity of detection, allowing for the study of increasingly smaller samples, and ( ii ) increase in the precision of isotopic analysis that allows more precise dating, the study of isotopic heterogeneity in the Solar System, and other studies. A variety of instrumental techniques are discussed, and important examples of discoveries are listed. Instrumental techniques and instruments include the ion microprobe, laser ablation gas MS, Auger EM, resonance ionization MS, accelerator MS, transmission EM, focused ion-beam microscopy, atom probe tomography, X-ray absorption near-edge structure/electron loss near-edge spectroscopy, Raman microprobe, NMR spectroscopy, and inductively coupled plasma MS.

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“…Cr isotope ratios to~1 % using power broadening to overcome small isotope shifts (~1 pm), the effects of Doppler broadening, and small pulse-to-pulse fluctuations in wavelength [14]. However, the isotope shift between uranium isotopes is much larger and the need to maximize the ratio of resonant to non-resonant ionization has prevented this approach from providing high precision in the measurement of isotope ratios.…”

Section: Success In Stabilizing Measuredmentioning

confidence: 99%

“…The time-dependent function of laser amplitude will create a time-dependent fraction of atoms participating in the interaction, therefore the ensemble of atoms as a whole will not behave coherently 1 . The experiments considered in this work will have a time-dependent pulse described by a Gaussian function with a FWHM of [10][11][12][13][14][15][16][17][18][19][20] ns. This is long compared to the time required for excitation to occur and therefore the experimental results will be considered in the limit of incoherent interactions.…”

Section: Resonant Excitation Of Discrete Transitions (Bound-bound)mentioning

confidence: 99%

“…RIMS uses photons tuned to atomic transitions to selectively excite and ionize neutral atoms vaporized from a sample while leaving other atomic species largely unionized [8,9]. RIMS is now routinely used for high-sensitivity and high-selectivity measurements of trace element and isotope composition in environmental [10,11,12] and extraterrestrial samples [13,14]. 1 The field of nuclear safeguards aims to ensure that the nuclear materials and processes used in nuclear power applications are not used the development of nuclear weapons.…”

Section: Introduction 11 Introductionmentioning

confidence: 99%

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Quantifying Uranium Isotope Ratios Using Resonance Ionization Mass Spectrometry: The Influence of Laser Parameters on Relative Ionization Probability

Isselhardt

2011

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Resonance Ionization Mass Spectrometry (RIMS) has been developed as a method to measure relative uranium isotope abundances. In this approach, RIMS is used as an elementselective ionization process to provide a distinction between uranium atoms and potential isobars without the aid of chemical purification and separation. We explore the laser parameters critical to the ionization process and their effects on the measured isotope ratio. Specifically, the use of broad bandwidth lasers with automated feedback control of wavelength was applied to the measurement of 235 U/ 238 U ratios to decrease laser-induced isotopic fractionation. By broadening the bandwidth of the first laser in a 3-color, 3-photon ionization process from a bandwidth of 1.8 GHz to about 10 GHz , the variation in sequential relative isotope abundance measurements decreased from >10% to less than 0.5%. This procedure was demonstrated for the direct interrogation of uranium oxide targets with essentially no sample preparation. A rate equation model for predicting the relative ionization probability has been developed to study the effect of variation in laser parameters on the measured isotope ratio. This work demonstrates that RIMS can be used for the robust measurement of uranium isotope ratios. Professor Stanley G. Prussin Dissertation Committee Chair iThis dissertation is dedicated to all those who have invested in me, especially my wife and son who have given the most.ii

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Resonance ionization mass spectrometry for precise measurements of isotope ratios

Cited by 47 publications

References 35 publications

RIMS analysis of ion induced fragmentation of molecules sputtered from an enriched U3O8 matrix

RIMS analysis of ion induced fragmentation of molecules sputtered from an enriched U3O8 matrix

Laboratory technology and cosmochemistry

Quantifying Uranium Isotope Ratios Using Resonance Ionization Mass Spectrometry: The Influence of Laser Parameters on Relative Ionization Probability

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