High-Resolution Fluorescence Spectra of Airborne Biogenic Secondary Organic Aerosols: Comparisons to Primary Biological Aerosol Particles and Implications for Single-Particle Measurements

Abstract. Measurements of primary biological aerosol particles, especially at altitudes relevant to cloud formation, are scarce. Single particle mass spectrometry (SPMS) has been used to probe aerosol chemical composition from ground and aircraft for over 20 years. Here we develop a method for identifying bioaerosols using SPMS. We show that identification of bioaerosol using SPMS is complicated because phosphorus-bearing mineral dust and phosphorus-rich combustion by-products such as fly ash produce mass spectra with peaks similar to those typically used as markers for bioaerosol. We have developed a methodology to differentiate and identify bioaerosol using machine learning statistical techniques applied to mass spectra of known particle types. This improved method provides far fewer false positives compared to approaches reported in the literature. The new method was then applied to ambient data collected at Storm Peak Laboratory to show that 0.04–0.3 % of particles in the 200–3000 nm aerodynamic diameter range were identified as bioaerosol.

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New application of direct analysis in real time high‐resolution mass spectrometry for the untargeted analysis of fresh and aged secondary organic aerosols generated from monoterpenes

Rapid Communications in Mass Spectrometry ◽

10.1002/rcm.8228 ◽

2018 ◽

Vol 33 (S1) ◽

pp. 50-59 ◽

Cited By ~ 1

Author(s):

Sébastien Schramm ◽

Nora Zannoni ◽

Valérie Gros ◽

Ralf Tillmann ◽

Astrid Kiendler‐Scharr ◽

...

Keyword(s):

Mass Spectrometry ◽

High Resolution ◽

Real Time ◽

Secondary Organic Aerosols ◽

High Resolution Mass Spectrometry ◽

Organic Aerosols ◽

Direct Analysis ◽

Untargeted Analysis ◽

High Resolution Mass ◽

Resolution Mass

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Improved identification of primary biological aerosol particles using single-particle mass spectrometry

Atmospheric Chemistry and Physics ◽

10.5194/acp-17-7193-2017 ◽

2017 ◽

Vol 17 (11) ◽

pp. 7193-7212 ◽

Cited By ~ 20

Author(s):

Maria A. Zawadowicz ◽

Karl D. Froyd ◽

Daniel M. Murphy ◽

Daniel J. Cziczo

Keyword(s):

Mass Spectrometry ◽

Single Particle ◽

Mass Spectra ◽

Mineral Dust ◽

Aerosol Particles ◽

Central Valley ◽

Particle Mass ◽

Cloud Formation ◽

Single Particle Mass Spectrometry ◽

Biological Aerosol Particles

Abstract. Measurements of primary biological aerosol particles (PBAP), especially at altitudes relevant to cloud formation, are scarce. Single-particle mass spectrometry (SPMS) has been used to probe aerosol chemical composition from ground and aircraft for over 20 years. Here we develop a method for identifying bioaerosols (PBAP and particles containing fragments of PBAP as part of an internal mixture) using SPMS. We show that identification of bioaerosol using SPMS is complicated because phosphorus-bearing mineral dust and phosphorus-rich combustion by-products such as fly ash produce mass spectra with peaks similar to those typically used as markers for bioaerosol. We have developed a methodology to differentiate and identify bioaerosol using machine learning statistical techniques applied to mass spectra of known particle types. This improved method provides far fewer false positives compared to approaches reported in the literature. The new method was then applied to two sets of ambient data collected at Storm Peak Laboratory and a forested site in Central Valley, California to show that 0.04–2 % of particles in the 200–3000 nm aerodynamic diameter range were identified as bioaerosol. In addition, 36–56 % of particles identified as biological also contained spectral features consistent with mineral dust, suggesting internal dust–biological mixtures.

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Applications of High-Resolution Electrospray Ionization Mass Spectrometry to Measurements of Average Oxygen to Carbon Ratios in Secondary Organic Aerosols

Environmental Science & Technology ◽

10.1021/es3017254 ◽

2012 ◽

Vol 46 (15) ◽

pp. 8315-8324 ◽

Cited By ~ 24

Author(s):

Adam P. Bateman ◽

Julia Laskin ◽

Alexander Laskin ◽

Sergey A. Nizkorodov

Keyword(s):

Mass Spectrometry ◽

High Resolution ◽

Electrospray Ionization ◽

Electrospray Ionization Mass Spectrometry ◽

Secondary Organic Aerosols ◽

Organic Aerosols ◽

Ionization Mass Spectrometry ◽

Ionization Mass

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Single-particle measurements of phase partitioning between primary and secondary organic aerosols

Faraday Discussions ◽

10.1039/c5fd00214a ◽

2016 ◽

Vol 189 ◽

pp. 31-49 ◽

Cited By ~ 9

Author(s):

Ellis Shipley Robinson ◽

Neil M. Donahue ◽

Adam T. Ahern ◽

Qing Ye ◽

Eric Lipsky

Keyword(s):

Single Particle ◽

Organic Molecules ◽

Secondary Organic Aerosols ◽

Large Fraction ◽

Organic Aerosols ◽

Organic Aerosol ◽

Urban Atmosphere ◽

Aerosol Formation ◽

Phase Partitioning ◽

Single Particle Mass Spectrometry

Organic aerosols provide a measure of complexity in the urban atmosphere. This is because the aerosols start as an external mixture, with many populations from varied local sources, that all interact with each other, with background aerosols, and with condensing vapors from secondary organic aerosol formation. The externally mixed particle populations start to evolve immediately after emission because the organic molecules constituting the particles also form thermodynamic mixtures – solutions – in which a large fraction of the constituents are semi-volatile. The external mixtures are thus well out of thermodynamic equilibrium, with very different activities for many constituents, and yet also have the capacity to relax toward equilibrium via gas-phase exchange of semi-volatile vapors. Here we describe experiments employing quantitative single-particle mass spectrometry designed to explore the extent to which various primary organic aerosol particle populations can interact with each other or with secondary organic aerosols representative of background aerosol populations. These methods allow us to determine when these populations will and when they will not mix with each other, and then to constrain the timescales for that mixing.

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