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Title: Effects of optical dopants and laser wavelength on atom probe tomography analyses of borosilicate glasses

Authors:
 [1];  [2]; ORCiD logo [2];  [2]; ORCiD logo [1]
  1. Department of Materials Science and Engineering, University of North Texas, Denton Texas
  2. Pacific Northwest National Laboratory, Richland Washington
Publication Date:
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1393680
Grant/Contract Number:
#13-5494; #DESC0016584
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Journal of the American Ceramic Society
Additional Journal Information:
Journal Volume: 100; Journal Issue: 10; Related Information: CHORUS Timestamp: 2017-09-21 02:53:12; Journal ID: ISSN 0002-7820
Publisher:
Wiley-Blackwell
Country of Publication:
United States
Language:
English

Citation Formats

Lu, Xiaonan, Schreiber, Daniel K., Neeway, James J., Ryan, Joseph V., and Du, Jincheng. Effects of optical dopants and laser wavelength on atom probe tomography analyses of borosilicate glasses. United States: N. p., 2017. Web. doi:10.1111/jace.14987.
Lu, Xiaonan, Schreiber, Daniel K., Neeway, James J., Ryan, Joseph V., & Du, Jincheng. Effects of optical dopants and laser wavelength on atom probe tomography analyses of borosilicate glasses. United States. doi:10.1111/jace.14987.
Lu, Xiaonan, Schreiber, Daniel K., Neeway, James J., Ryan, Joseph V., and Du, Jincheng. 2017. "Effects of optical dopants and laser wavelength on atom probe tomography analyses of borosilicate glasses". United States. doi:10.1111/jace.14987.
@article{osti_1393680,
title = {Effects of optical dopants and laser wavelength on atom probe tomography analyses of borosilicate glasses},
author = {Lu, Xiaonan and Schreiber, Daniel K. and Neeway, James J. and Ryan, Joseph V. and Du, Jincheng},
abstractNote = {},
doi = {10.1111/jace.14987},
journal = {Journal of the American Ceramic Society},
number = 10,
volume = 100,
place = {United States},
year = 2017,
month = 6
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on June 7, 2018
Publisher's Accepted Manuscript

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  • Atom probe tomography (APT) is a novel analytical microscopy method that provides three dimensional elemental mapping with sub-nanometer spatial resolution and has only recently been applied to insulating glass and ceramic samples. In this paper, we have studied the influence of the optical absorption in glass samples on APT characterization by introducing different transition metal optical dopants to a model borosilicate nuclear waste glass (international simple glass). A systematic comparison is presented of the glass optical properties and the resulting APT data quality in terms of compositional accuracy and the mass spectra quality for two APT systems: one with amore » green laser (532 nm, LEAP 3000X HR) and one with a UV laser (355 nm, LEAP 4000X HR). These data were also compared to the study of a more complex borosilicate glass (SON68). The results show that the analysis data quality such as compositional accuracy and total ions collected, was clearly linked to optical absorption when using a green laser, while for the UV laser optical doping aided in improving data yield but did not have a significant effect on compositional accuracy. Comparisons of data between the LEAP systems suggest that the smaller laser spot size of the LEAP 4000X HR played a more critical role for optimum performance than the optical dopants themselves. The smaller spot size resulted in more accurate composition measurements due to a reduced background level independent of the material’s optical properties.« less
  • The effects of laser wavelength (355 nm and 532 nm) and laser pulse energy on the quantitative accuracy of atom probe tomography (APT) examinations of LiFePO4 (LFP) are considered. A systematic investigation of ultraviolet (UV, 355 nm) and green (532 nm) laser assisted APT of LFP has revealed distinctly different behaviors. With the use of UV laser the major issue was identified as the preferential loss of oxygen (up to 10 at. %) while other elements (Li, Fe and P) were observed to be close to nominal ratios. Lowering the laser energy per pulse to 1 pJ increased the observedmore » oxygen concentration to near its correct stoichiometry and was well correlated with systematically higher concentrations of 16O2+ ions. This observation supports the premise that lower laser energies lead to a higher probability of oxygen molecule ionization. Conversely, at higher laser energies the resultant lower effective electric field reduces the probability of oxygen molecule ionization. Green laser assisted field evaporation led to the selective loss of Li (~50% deficiency) and correct ratios of the remaining elements, including the oxygen concentration. The loss of Li is explained by selective dc evaporation of lithium between laser pulses and relatively negligible oxygen loss as neutrals during green-laser pulsing. Lastly, plotting of multihit events on a Saxey plot for the straight-flight path data (green laser only) revealed a surprising dynamic recombination process for some molecular ions mid-flight.« less
  • The effects of laser wavelength (355 nm and 532 nm) and laser pulse energy on the quantitative analysis of LiFePO₄ by atom probe tomography are considered. A systematic investigation of ultraviolet (UV, 355 nm) and green (532 nm) laser assisted field evaporation has revealed distinctly different behaviors. With the use of a UV laser, the major issue was identified as the preferential loss of oxygen (up to 10 at%) while other elements (Li, Fe and P) were observed to be close to nominal ratios. Lowering the laser energy per pulse to 1 pJ/pulse from 50 pJ/pulse increased the observed oxygenmore » concentration to nearer its correct stoichiometry, which was also well correlated with systematically higher concentrations of ¹⁶O₂⁺ ions. Green laser assisted field evaporation led to the selective loss of Li (33% deficiency) and a relatively minor O deficiency. The loss of Li is likely a result of selective dc evaporation of Li between or after laser pulses. Comparison of the UV and green laser data suggests that the green wavelength energy was absorbed less efficiently than the UV wavelength because of differences in absorption at 355 and 532 nm for LiFePO₄. Plotting of multihit events on Saxey plots also revealed a strong neutral O₂ loss from molecular dissociation, but quantification of this loss was insufficient to account for the observed oxygen deficiency.« less