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Title: Effect of secondary organic aerosol coating thickness on the real-time detection and characterization of biomass-burning soot by two particle mass spectrometers

Biomass burning is a large source of light-absorbing refractory black carbon (rBC) particles with a wide range of morphologies and sizes. The net radiative forcing from these particles is strongly dependent on the amount and composition of non-light-absorbing material internally mixed with the rBC and on the morphology of the mixed particles. Understanding how the mixing state and morphology of biomass-burning aerosol evolves in the atmosphere is critical for constraining the influence of these particles on radiative forcing and climate. We investigated the response of two commercial laser-based particle mass spectrometers, the vacuum ultraviolet (VUV) ablation LAAPTOF and the IR vaporization SP-AMS, to monodisperse biomass-burning particles as we sequentially coated the particles with secondary organic aerosol (SOA) from α-pinene ozonolysis. We studied three mobility-selected soot core sizes, each with a number of successively thicker coatings of SOA applied. Using IR laser vaporization, the SP-AMS had different changes in sensitivity to rBC compared to potassium as a function of applied SOA coatings. We show that this is due to different effective beam widths for the IR laser vaporization region of potassium versus black carbon. The SP-AMS's sensitivity to black carbon (BC) mass was not observed to plateau following successive SOA coatings,more » despite achieving high OA : BC mass ratios greater than 9. We also measured the ion fragmentation pattern of biomass-burning rBC and found it changed only slightly with increasing SOA mass. The average organic matter ion signal measured by the LAAPTOF demonstrated a positive correlation with the condensed SOA mass on individual particles, despite the inhomogeneity of the particle core compositions. This demonstrates that the LAAPTOF can obtain quantitative mass measurements of aged soot-particle composition from realistic biomass-burning particles with complex morphologies and composition.« less
Authors:
 [1] ;  [1] ;  [1] ;  [2] ;  [3] ; ORCiD logo [1]
  1. Carnegie Mellon Univ., Pittsburgh, PA (United States). Center for Atmospheric Particle Studies
  2. Carnegie Mellon Univ., Pittsburgh, PA (United States); Penn State Greater Allegheny, McKeesport, PA (United States)
  3. Carnegie Mellon Univ., Pittsburgh, PA (United States). Center for Atmospheric Particle Studies)
Publication Date:
Grant/Contract Number:
SC0010121; CHE-1412309; AGS-1552608
Type:
Published Article
Journal Name:
Atmospheric Measurement Techniques (Online)
Additional Journal Information:
Journal Name: Atmospheric Measurement Techniques (Online); Journal Volume: 9; Journal Issue: 12; Journal ID: ISSN 1867-8548
Publisher:
European Geosciences Union
Research Org:
Carnegie Mellon Univ., Pittsburgh, PA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 09 BIOMASS FUELS
OSTI Identifier:
1337203
Alternate Identifier(s):
OSTI ID: 1358569

Ahern, Adam T., Subramanian, Ramachandran, Saliba, Georges, Lipsky, Eric M., Donahue, Neil M., and Sullivan, Ryan C.. Effect of secondary organic aerosol coating thickness on the real-time detection and characterization of biomass-burning soot by two particle mass spectrometers. United States: N. p., Web. doi:10.5194/amt-9-6117-2016.
Ahern, Adam T., Subramanian, Ramachandran, Saliba, Georges, Lipsky, Eric M., Donahue, Neil M., & Sullivan, Ryan C.. Effect of secondary organic aerosol coating thickness on the real-time detection and characterization of biomass-burning soot by two particle mass spectrometers. United States. doi:10.5194/amt-9-6117-2016.
Ahern, Adam T., Subramanian, Ramachandran, Saliba, Georges, Lipsky, Eric M., Donahue, Neil M., and Sullivan, Ryan C.. 2016. "Effect of secondary organic aerosol coating thickness on the real-time detection and characterization of biomass-burning soot by two particle mass spectrometers". United States. doi:10.5194/amt-9-6117-2016.
@article{osti_1337203,
title = {Effect of secondary organic aerosol coating thickness on the real-time detection and characterization of biomass-burning soot by two particle mass spectrometers},
author = {Ahern, Adam T. and Subramanian, Ramachandran and Saliba, Georges and Lipsky, Eric M. and Donahue, Neil M. and Sullivan, Ryan C.},
abstractNote = {Biomass burning is a large source of light-absorbing refractory black carbon (rBC) particles with a wide range of morphologies and sizes. The net radiative forcing from these particles is strongly dependent on the amount and composition of non-light-absorbing material internally mixed with the rBC and on the morphology of the mixed particles. Understanding how the mixing state and morphology of biomass-burning aerosol evolves in the atmosphere is critical for constraining the influence of these particles on radiative forcing and climate. We investigated the response of two commercial laser-based particle mass spectrometers, the vacuum ultraviolet (VUV) ablation LAAPTOF and the IR vaporization SP-AMS, to monodisperse biomass-burning particles as we sequentially coated the particles with secondary organic aerosol (SOA) from α-pinene ozonolysis. We studied three mobility-selected soot core sizes, each with a number of successively thicker coatings of SOA applied. Using IR laser vaporization, the SP-AMS had different changes in sensitivity to rBC compared to potassium as a function of applied SOA coatings. We show that this is due to different effective beam widths for the IR laser vaporization region of potassium versus black carbon. The SP-AMS's sensitivity to black carbon (BC) mass was not observed to plateau following successive SOA coatings, despite achieving high OA : BC mass ratios greater than 9. We also measured the ion fragmentation pattern of biomass-burning rBC and found it changed only slightly with increasing SOA mass. The average organic matter ion signal measured by the LAAPTOF demonstrated a positive correlation with the condensed SOA mass on individual particles, despite the inhomogeneity of the particle core compositions. This demonstrates that the LAAPTOF can obtain quantitative mass measurements of aged soot-particle composition from realistic biomass-burning particles with complex morphologies and composition.},
doi = {10.5194/amt-9-6117-2016},
journal = {Atmospheric Measurement Techniques (Online)},
number = 12,
volume = 9,
place = {United States},
year = {2016},
month = {12}
}