Preprints
https://doi.org/10.5194/ar-2023-21
https://doi.org/10.5194/ar-2023-21
04 Jan 2024
 | 04 Jan 2024
Status: a revised version of this preprint was accepted for the journal AR and is expected to appear here in due course.

A multi-instrumental approach for calibrating two real-time mass spectrometers using high performance liquid chromatography and positive matrix factorization

Melinda K. Schueneman, Doug A. Day, Dongwook Kim, Pedro Campuzano-Jost, Seonsik Yun, Marla P. DeVault, Anna C. Ziola, Paul J. Ziemann, and Jose L. Jimenez

Abstract. Obtaining quantitative information from real-time soft-ionization aerosol instruments such as an Extractive Electrospray time-of-flight Mass Spectrometer (EESI) can be challenging, due to many individual species having different, and often hard to predict, sensitivities. Directly calibrating is time-consuming and relevant standards are often hard to obtain. In addition, the molecular identities of many of the sampled species may be ambiguous. Bulk OA sensitivities are sometimes used to estimate molecular sensitivities, but different types of OA can have bulk sensitivities that vary by a factor of ~10. A system to separate the compounds present in complex samples can enable their direct calibration. Here, high performance liquid chromatography (HPLC) followed by aerosol formation via atomization was combined with online, 1 Hz measurements to calibrate the EESI and a High Resolution Aerosol Mass Spectrometer (AMS) for compounds present in a secondary organic aerosol (SOA) mixture. Pure compounds were used to test the method and characterize its uncertainties. Pure compound calibration factors were consistent within ±20 % for direct atomization vs. HPLC separation, which is far superior to the orders of magnitude sensitivity differences that are possible with EESI. For species that were not well separated by chromatography, Positive Matrix Factorization (PMF) based on AMS spectra was used to test its ability to separate overlapping species. In two test cases, further separation was achieved using PMF, but derived sensitivities from direct and HPLC calibrations varied by up to a factor of 2.

Melinda K. Schueneman, Doug A. Day, Dongwook Kim, Pedro Campuzano-Jost, Seonsik Yun, Marla P. DeVault, Anna C. Ziola, Paul J. Ziemann, and Jose L. Jimenez

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on ar-2023-21', Anonymous Referee #1, 27 Jan 2024
  • RC2: 'Comment on ar-2023-21', Anonymous Referee #2, 30 Jan 2024
  • AC1: 'Comment on ar-2023-21', Melinda Schueneman, 01 Apr 2024

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on ar-2023-21', Anonymous Referee #1, 27 Jan 2024
  • RC2: 'Comment on ar-2023-21', Anonymous Referee #2, 30 Jan 2024
  • AC1: 'Comment on ar-2023-21', Melinda Schueneman, 01 Apr 2024
Melinda K. Schueneman, Doug A. Day, Dongwook Kim, Pedro Campuzano-Jost, Seonsik Yun, Marla P. DeVault, Anna C. Ziola, Paul J. Ziemann, and Jose L. Jimenez
Melinda K. Schueneman, Doug A. Day, Dongwook Kim, Pedro Campuzano-Jost, Seonsik Yun, Marla P. DeVault, Anna C. Ziola, Paul J. Ziemann, and Jose L. Jimenez

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Short summary
Here, we present a new analytical technique for making atmospheric aerosol measurements quantitative. We include information on calibrating two aerosol chemical instruments using liquid chromatography combined with statistical component analysis. We validate the method through the testing of standards and complex mixtures, which shows promising results.
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