scholarly journals High efficiency laser resonance ionization of plutonium

2021 ◽  
Vol 11 (1) ◽  
Author(s):  
Alfredo Galindo-Uribarri ◽  
Yuan Liu ◽  
Elisa Romero Romero ◽  
Daniel W. Stracener

AbstractThree-step resonance photoionization spectra of plutonium have been studied with Ti:Sapphire lasers for the development of efficient laser ionization schemes for ultra-trace analysis of Pu isotopes by resonance ionization mass spectrometry. We observed eighteen intermediate excited states of even parity in the energy range 35568–36701 $${\text {cm}}^{-1}$$ cm - 1 , thirteen of them have not been previously documented, and a larger number of high-lying excited states and autoionizing states of odd-parity between 48238 and 49510 $${\text {cm}}^{-1}$$ cm - 1 . Three-color, three-photon ionization schemes via six intermediate states were evaluated under similar ion source operating conditions. This led to a highly efficient three-step scheme with an overall ionization efficiency of $$51.1 \pm 1.3\%$$ 51.1 ± 1.3 % , which is an order of magnitude improvement over the previously reported ionization efficiency for Pu.

2019 ◽  
Vol 107 (7) ◽  
pp. 645-652 ◽  
Author(s):  
Sebastian Raeder ◽  
Nina Kneip ◽  
Tobias Reich ◽  
Dominik Studer ◽  
Norbert Trautmann ◽  
...  

Abstract Resonance ionization mass spectrometry is an efficient tool to detect minute amounts of long-lived radio-isotopes in environmental samples. Applying resonant excitation and ionization with pulsed laser radiation within a hot cavity atomizer enables the sensitive detection and precise quantification of long-lived actinide isotopes. Due to the inherently element selective ionization process, this method ensures ultimate suppression of contaminations from other elements and molecules. The characterization of in-source resonance ionization of the actinide elements U, Th, Np, and Am using a compact quadrupole mass spectrometer (QMS) setup are discussed.


2021 ◽  
Author(s):  
Chenyang Bi ◽  
Jordan E. Krechmer ◽  
Manjula R. Canagaratna ◽  
Gabriel Isaacman-VanWertz

Abstract. Quantitative calibration of analytes using chemical ionization mass spectrometers (CIMS) has been hindered by the lack of commercially available standards of atmospheric oxidation products. To accurately calibrate analytes without standards, techniques have been recently developed to log-linearly correlate analyte sensitivity with instrument operating conditions. However, there is an inherent bias when applying log-linear calibration relationships that is typically ignored. In this study, we examine the bias in a log-linear based calibration curve based on prior mathematical work. We quantify the potential bias within the context of a CIMS-relevant relationship between analyte sensitivity and instrument voltage differentials. Uncertainty in three parameters has the potential to contribute to the bias, specifically the inherent extent to which the nominal relationship can capture true sensitivity, the slope of the relationship, and the voltage differential below which maximum sensitivity is achieved. Using a prior published case study, we estimate an average bias of 30%, with one order of magnitude for less sensitive compounds in some circumstances. A parameter-explicit solution is proposed in this work for completely removing the inherent bias generated in the log-linear calibration relationships. A simplified correction method is also suggested for cases where a comprehensive bias correction is not possible due to unknown uncertainties of calibration parameters, which is shown to eliminate the bias on average but not for each individual compound.


2021 ◽  
Vol 14 (10) ◽  
pp. 6551-6560
Author(s):  
Chenyang Bi ◽  
Jordan E. Krechmer ◽  
Manjula R. Canagaratna ◽  
Gabriel Isaacman-VanWertz

Abstract. Quantitative calibration of analytes using chemical ionization mass spectrometers (CIMSs) has been hindered by the lack of commercially available standards of atmospheric oxidation products. To accurately calibrate analytes without standards, techniques have been recently developed to log-linearly correlate analyte sensitivity with instrument operating conditions. However, there is an inherent bias when applying log-linear calibration relationships that is typically ignored. In this study, we examine the bias in a log-linear-based calibration curve based on prior mathematical work. We quantify the potential bias within the context of a CIMS-relevant relationship between analyte sensitivity and instrument voltage differentials. Uncertainty in three parameters has the potential to contribute to the bias, specifically the inherent extent to which the nominal relationship can capture true sensitivity, the slope of the relationship, and the voltage differential below which maximum sensitivity is achieved. Using a prior published case study, we estimate an average bias of 30 %, with 1 order of magnitude for less sensitive compounds in some circumstances. A parameter-explicit solution is proposed in this work for completely removing the inherent bias generated in the log-linear calibration relationships. A simplified correction method is also suggested for cases where a comprehensive bias correction is not possible due to unknown uncertainties of calibration parameters, which is shown to eliminate the bias on average but not for each individual compound.


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