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

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. Here, 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.
Authors:
 [1] ;  [2] ;  [3] ;  [4]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Earth, Atmospheric and Planetary Sciences
  2. National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States). Chemical Sciences Division; Univ. of Colorado, Boulder, CO (United States). Cooperative Inst. for Research in Environmental Sciences
  3. National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States). Chemical Sciences Division
  4. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Earth, Atmospheric and Planetary Sciences; Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Civil and Environmental Engineering
Publication Date:
Grant/Contract Number:
SC0014487; NNX13AO15G; AGS-1461347; AGS-1339264
Type:
Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 17; Journal Issue: 11; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Research Org:
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES
OSTI Identifier:
1364084
Alternate Identifier(s):
OSTI ID: 1425937

Zawadowicz, Maria A., Froyd, Karl D., Murphy, Daniel M., and Cziczo, Daniel J.. Improved identification of primary biological aerosol particles using single-particle mass spectrometry. United States: N. p., Web. doi:10.5194/acp-17-7193-2017.
Zawadowicz, Maria A., Froyd, Karl D., Murphy, Daniel M., & Cziczo, Daniel J.. Improved identification of primary biological aerosol particles using single-particle mass spectrometry. United States. doi:10.5194/acp-17-7193-2017.
Zawadowicz, Maria A., Froyd, Karl D., Murphy, Daniel M., and Cziczo, Daniel J.. 2017. "Improved identification of primary biological aerosol particles using single-particle mass spectrometry". United States. doi:10.5194/acp-17-7193-2017.
@article{osti_1364084,
title = {Improved identification of primary biological aerosol particles using single-particle mass spectrometry},
author = {Zawadowicz, Maria A. and Froyd, Karl D. and Murphy, Daniel M. and Cziczo, Daniel J.},
abstractNote = {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. Here, 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.},
doi = {10.5194/acp-17-7193-2017},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 11,
volume = 17,
place = {United States},
year = {2017},
month = {6}
}