Preprints
https://doi.org/10.5194/egusphere-2023-2610
https://doi.org/10.5194/egusphere-2023-2610
04 Dec 2023
 | 04 Dec 2023

Technical note: Determining chemical composition of atmospheric single particles by a standard-free mass calibration algorithm

Shao Shi, Jinghao Zhai, Xin Yang, Yechun Ruan, Yuanlong Huang, Xujian Chen, Antai Zhang, Jianhuai Ye, Guomao Zheng, Baohua Cai, Yaling Zeng, Yixiang Wang, Chunbo Xing, Yujie Zhang, Tzung-May Fu, Lei Zhu, Huizhong Shen, and Chen Wang

Abstract. The chemical composition of individual particles can be revealed by single particle mass spectrometers (SPMS). With higher accuracy in the ratio of mass to charge (m/z), more detailed chemical information could be obtained. In the SPMS, the conventional standard-based calibration methods (internal/external) are constrained by the inhomogeneity of ionization lasers and the finite focusing ability of the inlet system, etc., therefore, the mass accuracy is restricted. In this study, we obtained the detailed and trustable chemical composition of single particles utilizing a standard-free mass calibration algorithm. In the algorithm, the characteristic distributions of hundreds of ions were concluded and collected in a database denoted as prototype. Each single-particle mass spectrum was tentatively calibrated by a mass calibration function with specific coefficients. The range of coefficients is constrained by the magnitude of mass deviation to a finite vector space. To find the optimal coefficient vector, the conformity of each tentatively calibrated spectrum to the prototype dataset was assessed. With maximum conformity, the optimal calibrated spectrum was obtained. For more than 98 % ambient particles, a twentyfold improvement in mass accuracy, from ~10,000 ppm (integer) to ~500 ppm (2 decimal places) was achieved. The improved mass accuracy validated the determination of adjacent ions with m/z difference ~0.05 Th. Furthermore, atmospheric trace ions that were poorly studied before are successfully specified. The obtained detailed single-particle-level chemical information could help understand the source apportionment, reaction mechanism, and mixing state of atmospheric particles.

Shao Shi, Jinghao Zhai, Xin Yang, Yechun Ruan, Yuanlong Huang, Xujian Chen, Antai Zhang, Jianhuai Ye, Guomao Zheng, Baohua Cai, Yaling Zeng, Yixiang Wang, Chunbo Xing, Yujie Zhang, Tzung-May Fu, Lei Zhu, Huizhong Shen, and Chen Wang

Status: final response (author comments only)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on egusphere-2023-2610', Anonymous Referee #1, 22 Dec 2023
  • RC2: 'Comment on egusphere-2023-2610', Anonymous Referee #2, 13 Feb 2024
Shao Shi, Jinghao Zhai, Xin Yang, Yechun Ruan, Yuanlong Huang, Xujian Chen, Antai Zhang, Jianhuai Ye, Guomao Zheng, Baohua Cai, Yaling Zeng, Yixiang Wang, Chunbo Xing, Yujie Zhang, Tzung-May Fu, Lei Zhu, Huizhong Shen, and Chen Wang
Shao Shi, Jinghao Zhai, Xin Yang, Yechun Ruan, Yuanlong Huang, Xujian Chen, Antai Zhang, Jianhuai Ye, Guomao Zheng, Baohua Cai, Yaling Zeng, Yixiang Wang, Chunbo Xing, Yujie Zhang, Tzung-May Fu, Lei Zhu, Huizhong Shen, and Chen Wang

Viewed

Total article views: 323 (including HTML, PDF, and XML)
HTML PDF XML Total Supplement BibTeX EndNote
239 64 20 323 33 12 10
  • HTML: 239
  • PDF: 64
  • XML: 20
  • Total: 323
  • Supplement: 33
  • BibTeX: 12
  • EndNote: 10
Views and downloads (calculated since 04 Dec 2023)
Cumulative views and downloads (calculated since 04 Dec 2023)

Viewed (geographical distribution)

Total article views: 304 (including HTML, PDF, and XML) Thereof 304 with geography defined and 0 with unknown origin.
Country # Views %
  • 1
1
 
 
 
 
Latest update: 29 Feb 2024
Download
Short summary
The determination of ions in the mass spectra of individual particles remains uncertain. We have developed a standard-free mass calibration algorithm applicable to more than 98 % of ambient particles. With our algorithm, ions with ~0.05 Th mass difference could be determined. Therefore, many more atmospheric species could be determined and involved in the source apportionment of aerosols, the study of chemical reaction mechanisms, and the analysis of single-particle mixing states.