Measurement of boron isotopic ratio with non-gated molecular spectroscopy of femtosecond laser-produced plasma

Yee, Ben C.; Hartig, Kyle C.; Ko, Phyllis; McNutt, Jessica; Jovanovic, Igor

doi:10.1016/j.sab.2012.12.003

Cited by 19 publications

(15 citation statements)

References 19 publications

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“…Recent introduction of the femtosecond LAMIS [39,40] indicated further prospects for improving accuracy and sensitivity in this technique. Femtosecond ablation atomizes materials better than nanosecond pulses do, thus reducing chances for unwanted fractionation effects.…”

Section: Resultsmentioning

confidence: 99%

Laser ablation molecular isotopic spectrometry of carbon isotopes

Bol’shakov

Mao

Jain

et al. 2015

Spectrochimica Acta Part B: Atomic Spectroscopy

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Quantitative determination of carbon isotopes using Laser Ablation Molecular Isotopic Spectrometry (LAMIS) is described. Optical emission of diatomic molecules CN and C 2 is used in these measurements. Two quantification approaches are presented: empirical calibration of spectra using a set of reference standards and numerical fitting of a simulated spectrum to the experimental one. Formation mechanisms of C 2 and CN in laser ablation plasma are briefly reviewed to provide insights for implementation of LAMIS measurements. A simulated spectrum of the 12 C 2 Swan system was synthesized using four constituents within 473.5-476.5 nm.Simulation included three branches of 12 C 2 (1-0), branches R(0-0) and R(1-1), and branch P(9-8) of 12 C 2 . Spectral positions of the tail lines in R(0-0) and R(1-1) were experimentally measured, since they were not accurately known before. The Swan band (1-0) of the isotopologue 13 C 12 C was also simulated. Fitting to the experimental spectrum yielded the ratio 13 C/ 12 C = 1.08% in a © 2015. This manuscript version is made available under the Elsevier user license http://www.elsevier.com/open-access/userlicense/1.0/ good agreement with measurements by isotope ratio mass spectrometry. LAMIS promises to be useful in coal, oil and shale exploration, carbon sequestration monitoring, and agronomy studies.

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Section: Resultsmentioning

confidence: 99%

Laser ablation molecular isotopic spectrometry of carbon isotopes

Bol’shakov

Mao

Jain

et al. 2015

Spectrochimica Acta Part B: Atomic Spectroscopy

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“…The reported precisions, expressed as standard deviations of the percentage compositions of 11 B, ranged from 0.9 to 3.7% for a boron-nitride solid sample at natural isotopic abundance. Jovanovic and co-workers [8,9] also performed LAMIS of boron but with a femtosecond laser, and reported precisions ~ 1.9 to 3.0% on the measured isotopic composition. Sarkar et al [10] advanced the analytical capabilities of LAMIS for boron isotopic analysis through a detailed characterization of the factors limiting the analytical accuracy and precision, and found that a critical factor is the data-pretreatment procedure to remove shot-toshot spectral variations prior to partial least square (PLS) regression.…”

Section: Introductionmentioning

confidence: 99%

“…In all the above examples, the minor isotopes were present at relatively high abundances. The boron figures quoted above were all from boron samples with natural isotopic 5 abundance [2,3,[7][8][9][10] (the minor isotope, 10 B is ~ 19.9% [12]) whereas the atom percentages of 2 H in the OH/OD LAMIS study [11] ranged from 6% to 97%. There are many isotopes with natural abundances around or less than 1% (e.g., 13 C ~1.1%, 15 N ~0.4%, 18 O ~0.2%, 235 U ~0.7% [12]).…”

Section: Introductionmentioning

confidence: 99%

Reduction of spectral interferences and noise effects in laser ablation molecular isotopic spectrometry with partial least square regression – a computer simulation study

Mao

Chan

Zorba

et al. 2016

Spectrochimica Acta Part B: Atomic Spectroscopy

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The fundamental analytical accuracies and precisions attainable by laser ablation molecular isotopic spectrometry (LAMIS), with emphasis on the impacts from spectral interferences and measurement noise, were investigated by means of computer simulation. The study focused on the analysis of a minor isotope at sub-to single-percentage abundance level. With a natural abundance about 1.1% for 13 C, the C 2 Swan band (d 3 Π ga 3 Π u) with  = +1 was selected as a representative system. The characteristics (e.g., noise amplitude and distribution, signal strength, and signal-to-background ratio) of the simulated spectra were experimentally characterized. Partial least square (PLS) regression was used to extract isotopic information from the simulated molecular spectra. In the absence of any spectral interference and with the use of a calibration set consisting of eleven isotopic standards, the theoretical accuracies and precisions with signal accumulation from 100 laser shots are about 0.002% and 0.001%, respectively, in absolute percentage abundance of 13 C. The theoretical analytical accuracies slightly degrade, but are adequate for many applications, to 0.004% and 0.008% respectively, for calibrations involving only three and two isotopic standards. It was found that PLS regression is not only immune to both source-flicker and photon-shot noise, but is also effective in differentiating the spectral patterns from the analyte against those from spectral interferences. The influences of spectral interference from single or multiple atomic emission lines were simulated, and new ways to minimize their impacts were formulated and demonstrated. It was found that the wavelength range selected for the computation of the normalization factor should not contain any spectralinterfering peak, and a properly chosen wavelength range increases the tolerance of spectral interference by at least one order of magnitude. With matrix-matched calibration standards, the precisions (expressed as RSDs of the determined 13 C isotopic abundances) degrade from ~1‰ in 2 the absence of spectral interference, to ~3‰, 10‰ and 20‰ with spectral-interfering peaks that are 10, 100 and 1000, respectively, stronger than the molecular bandhead of the analyte. The study concluded that PLS regression is a powerful and indispensable tool for extraction of isotopic information from LAMIS spectra.

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“…These limitations are not always compatible with remote measurements. In the recently developed technique of Laser Ablation Molecular Isotopic Spectrometry (LAMIS)212223, radiative molecular transitions from diatomic molecules are used to extract the isotopic composition of a sample under ambient atmospheric conditions. A similar method has been demonstrated in earlier work by Niki et al 24,.…”

mentioning

confidence: 99%

Standoff Detection of Uranium and its Isotopes by Femtosecond Filament Laser Ablation Molecular Isotopic Spectrometry

Hartig

Ghebregziabher

Jovanovic

2017

Sci Rep

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The ability to perform not only elementally but also isotopically sensitive detection and analysis at standoff distances is impor-tant for remote sensing applications in diverse ares, such as nuclear nonproliferation, environmental monitoring, geophysics, and planetary science. We demonstrate isotopically sensitive real-time standoff detection of uranium by the use of femtosecond filament-induced laser ablation molecular isotopic spectrometry. A uranium oxide molecular emission isotope shift of 0.05 ± 0.007 nm is reported at 593.6 nm. We implement both spectroscopic and acoustic diagnostics to characterize the properties of uranium plasma generated at different filament-uranium interaction points. The resulting uranium oxide emis-sion exhibits a nearly constant signal-to-background ratio over the length of the filament, unlike the uranium atomic and ionic emission, for which the signal-to-background ratio varies significantly along the filament propagation. This is explained by the different rates of increase of plasma density and uranium oxide density along the filament length resulting from spectral and temporal evolution of the filament along its propagation. The results provide a basis for the optimal use of filaments for standoff detection and analysis of uranium isotopes and indicate the potential of the technique for a wider range of remote sensing applications that require isotopic sensitivity.

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Measurement of boron isotopic ratio with non-gated molecular spectroscopy of femtosecond laser-produced plasma

Cited by 19 publications

References 19 publications

Laser ablation molecular isotopic spectrometry of carbon isotopes

Laser ablation molecular isotopic spectrometry of carbon isotopes

Reduction of spectral interferences and noise effects in laser ablation molecular isotopic spectrometry with partial least square regression – a computer simulation study

Standoff Detection of Uranium and its Isotopes by Femtosecond Filament Laser Ablation Molecular Isotopic Spectrometry

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