An intercomparison study of four different techniques for measuring the chemical composition of nanoparticles
- Creators
- Caudillo, Lucía
- Surdu, Mihnea
- Lopez, Brandon
- Wang, Mingyi
- Thoma, Markus
- Bräkling, Steffen
- Buchholz, Angela
- Simon, Mario
- Wagner, Andrea C.
- Müller, Tatjana
- Granzin, Manuel
- Heinritzi, Martin
- Amorim, Antonio
- Bell, David M.
- Brasseur, Zoé
- Dada, Lubna
- Duplissy, Jonathan
- Finkenzeller, Henning
- He, Xu-Cheng
- Lamkaddam, Houssni
- Mahfouz, Naser G. A.
- Makhmutov, Vladimir
- Manninen, Hanna E.
- Marie, Guillaume
- Marten, Ruby
- Mauldin, Roy L.
- Mentler, Bernhard
- Onnela, Antti
- Petäjä, Tuukka
- Pfeifer, Joschka
- Philippov, Maxim
- Piedehierro, Ana A.
- Rörup, Birte
- Scholz, Wiebke
- Shen, Jiali
- Stolzenburg, Dominik
- Tauber, Christian
- Tian, Ping
- Tomé, António
- Umo, Nsikanabasi Silas
- Wang, Dongyu S.
- Wang, Yonghong
- Weber, Stefan K.
- Welti, André
- Zauner-Wieczorek, Marcel
- Baltensperger, Urs
- Flagan, Richard C.
- Hansel, Armin
- Kirkby, Jasper
- Kulmala, Markku
- Lehtipalo, Katrianne
- Worsnop, Douglas R.
- El Haddad, Imad
- Donahue, Neil M.
- Vogel, Alexander L.
- Kürten, Andreas
- Curtius, Joachim
Abstract
Abstract. Currently, the complete chemical characterization of nanoparticles (< 100 nm) represents an analytical challenge, since these particles are abundant in number but have negligible mass. Several methods for particle-phase characterization have been recently developed to better detect and infer more accurately the sources and fates of sub-100 nm particles, but a detailed comparison of different approaches is missing. Here we report on the chemical composition of secondary organic aerosol (SOA) nanoparticles from experimental studies of α-pinene ozonolysis at −50, −30, and −10 °C and intercompare the results measured by different techniques. The experiments were performed at the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN). The chemical composition was measured simultaneously by four different techniques: (1) thermal desorption–differential mobility analyzer (TD–DMA) coupled to a NO⁻₃ chemical ionization–atmospheric-pressure-interface–time-of-flight (CI–APi–TOF) mass spectrometer, (2) filter inlet for gases and aerosols (FIGAERO) coupled to an I⁻ high-resolution time-of-flight chemical ionization mass spectrometer (HRToF-CIMS), (3) extractive electrospray Na⁺ ionization time-of-flight mass spectrometer (EESI-TOF), and (4) offline analysis of filters (FILTER) using ultra-high-performance liquid chromatography (UHPLC) and heated electrospray ionization (HESI) coupled to an Orbitrap high-resolution mass spectrometer (HRMS). Intercomparison was performed by contrasting the observed chemical composition as a function of oxidation state and carbon number, by estimating the volatility and comparing the fraction of volatility classes, and by comparing the thermal desorption behavior (for the thermal desorption techniques: TD–DMA and FIGAERO) and performing positive matrix factorization (PMF) analysis for the thermograms. We found that the methods generally agree on the most important compounds that are found in the nanoparticles. However, they do see different parts of the organic spectrum. We suggest potential explanations for these differences: thermal decomposition, aging, sampling artifacts, etc. We applied PMF analysis and found insights of thermal decomposition in the TD–DMA and the FIGAERO.
Additional Information
© Author(s) 2023. This work is distributed under the Creative Commons Attribution 4.0 License. We thank CERN for providing the CLOUD facility to perform the experiments and the CLOUD community for supporting this study. We especially would like to thank Katja Ivanova, Timo Keber, Frank Malkemper, Robert Sitals, Hanna Elina Manninen, Antti Onnela, and Robert Kristic for their contributions to the experiment. This research has been supported by the Horizon 2020 research and innovation program (CLOUD-MOTION, grant no. 764991, and PSI-FELLOW-II-3i, grant no. 701647); the Bundesministerium für Bildung, Wissenschaft, Forschung und Technologie (CLOUD-16, grant no. 01LK1601A); the Deutsche Forschungsgemeinschaft (grant no. 410009325); the National Science Foundation (grant nos. AGS-1801280, AGS-1801574, AGS-1801897, AGS-1602086, and AGS-18801329); the Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung (grant nos. 200020_172602 and 20FI20_172622); CERN (grant no. CERN/FIS-COM/0028/2019); the Academy of Finland (grant nos. 325656, 316114, 314798, 325647, 341349, and 337549); the European Research Council, HORIZON EUROPE (ATM-GTP, grant no. 742206); and the Prince Albert II of Monaco Foundation (grant no. 2859). Author contributions LC, MS, BL, MW, SB, TM, MG, ZB, LD, JD, HF, XCH, HL, NGAM, VM, HEM, GM, RM, RLM, BM, AO, TP, JP, MP, AAP, BR, WS, JS, PT, AT, NSU, DSW, SKW, ACW, WY, MZW, UB, JK, MK, KL, IEH, NMD, AK, and JC prepared the CLOUD facility and measurement instruments. LC, MS, BL, MW, SB, TM, MG, AA, DMB, LD, JD, HF, XCH, HL, NGAM, VM, GM, RLM, BM, JS, CT, AT, NSU, DSW, SKW, MZW, and JK collected the data. LC, MS, BL, MW, MT, SB, AB, SKW, and JC analyzed the data. LC, MS, BL, MW, MT, AB, MSim, ACW, MH, DMB, LD, TP, DS, RCF, AH, MK, KL, DW, IEH, NMD, ALV, AK, and JC contributed to the scientific discussion and interpretation of the results. LC, AB, UB, RCF, and JC contributed to the writing of the manuscript. Data availability. Data related to this article are available upon reasonable request to the corresponding authors. The supplement related to this article is available online at: https://doi.org/10.5194/acp-23-6613-2023-supplement.Attached Files
Published - acp-23-6613-2023.pdf
Supplemental Material - acp-23-6613-2023-supplement.pdf
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Additional details
- Eprint ID
- 122129
- Resolver ID
- CaltechAUTHORS:20230705-942391700.13
- 764991
- Marie Curie Fellowship
- 701647
- Marie Curie Fellowship
- 01LK1601A
- Bundesministerium für Bildung, Wissenschaft, Forschung und Technologie (BMBF)
- 410009325
- Deutsche Forschungsgemeinschaft (DGF)
- AGS-1801280
- NSF
- AGS-1801574
- NSF
- AGS-1801897
- NSF
- AGS-1602086
- NSF
- 200020_172602
- Swiss National Science Foundation (SNSF)
- 20FI20_172622
- Swiss National Science Foundation (SNSF)
- CERN/FIS-COM/0028/2019
- CERN
- 325656
- Academy of Finland
- 316114
- Academy of Finland
- 314798
- Academy of Finland
- 325647
- Academy of Finland
- 341349
- Academy of Finland
- 337549
- Academy of Finland
- 742206
- European Research Council (ERC)
- 2859
- Prince Albert II of Monaco Foundation
- Created
-
2023-07-26Created from EPrint's datestamp field
- Updated
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2023-07-26Created from EPrint's last_modified field