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Atmospheric Measurement Techniques An interactive open-access journal of the European Geosciences Union
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https://doi.org/10.5194/amt-2019-489
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/amt-2019-489
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 09 Mar 2020

Submitted as: research article | 09 Mar 2020

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This preprint is currently under review for the journal AMT.

Development of an Automatic Linear Calibration Method for High Resolution Single Particle Mass Spectrometry: Improved Chemical Species Identification for Atmospheric Aerosols

Shengqiang Zhu1, Lei Li2, Shurong Wang1, Mei Li2, Yaxi Liu1, Xiaohui Lu1, Hong Chen1, Lin Wang1,3, Jianmin Chen1,3, Zhou Zhen2, Xin Yang1,3, and Xiaofei Wang1,3 Shengqiang Zhu et al.
  • 1Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan University, Shanghai 11200433, China
  • 2Institute of Mass Spectrometer and Atmospheric Environment, Jinan University, Guangzhou, 510632, China
  • 3Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China

Abstract. The mass resolution of laser desorption ionization (LDI) single particle aerosol mass spectrometry (SPAMS) is usually low (~500), which has been greatly improved by recent development of delayed ion extraction technique. However, due to large fluctuations among LDI processes during each laser shot, accurate calibration of mass-to-charge ratio for high resolution SPAMS spectra is challenging. Here we developed an automatic linear calibration method to improve the accuracy of mass-to-charge (m/z) measurement for single atmospheric aerosol particles. Laboratory generated sea spray aerosol and atmospheric ambient aerosol were tested. After the calibration, the fluctuation ranges of the reference ions (e.g. Pb+ and SO4+) m/z reaches ±0.018 for sea spray aerosol and ±0.024 for ambient aerosol in average mass spectra. With such m/z accuracy, the HR-SPAMS spectra of sea spray aerosol can easily identify elemental compositions of organic peaks, such as Cx, CxHy and CxHyOz. While the chemical compositions of ambient aerosols are more complicated, CxHy, CxHyOz and CNO peaks can also be identified based on their accurate mass. With the improved resolution, the time series of peaks with small m/z differences can be separated and measured. In addition, it is also found that applying high resolution data with enhanced mass calibration can significantly affect particle classification (identification) using the ART-2a algorism, which classify particles based on similarities among single particle mass spectra.

Shengqiang Zhu et al.

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Short summary
Single Particle Aerosol Mass Spectrometer (SPAMS) has been widely used to detect chemical compositions and sizes of individual aerosol particles. However, it has a major issue: the mass accuracy of HR-SPAMS is low. Here we developed an automatic linear calibration method to greatly improve the mass accuracy of SPAMS spectra so that the elemental compositions of organic peaks, such as Cx, CxHy, CxHyOz and CxHyNO peaks can be directly identified just based on their m/z values.
Single Particle Aerosol Mass Spectrometer (SPAMS) has been widely used to detect chemical...
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