Chemistry of new particle growth in mixed urban and biogenic emissions – insights from CARES

Regional new particle formation and growth events (NPEs) were observed on most days over the Sacramento and western Sierra foothills area of California in June 2010 during the Carbonaceous Aerosols and Radiative Effect Study (CARES). Simultaneous particle measurements at both the T0 (Sacramento, urb...

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Main Authors: A. Setyan, C. Song, M. Merkel, W. B. Knighton, T. B. Onasch, M. R. Canagaratna, D. R. Worsnop, A. Wiedensohler, J. E. Shilling, Q. Zhang
Format: Article
Language:English
Published: Copernicus Publications 2014-07-01
Series:Atmospheric Chemistry and Physics
Online Access:http://www.atmos-chem-phys.net/14/6477/2014/acp-14-6477-2014.pdf
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author A. Setyan
C. Song
M. Merkel
W. B. Knighton
T. B. Onasch
M. R. Canagaratna
D. R. Worsnop
A. Wiedensohler
J. E. Shilling
Q. Zhang
author_facet A. Setyan
C. Song
M. Merkel
W. B. Knighton
T. B. Onasch
M. R. Canagaratna
D. R. Worsnop
A. Wiedensohler
J. E. Shilling
Q. Zhang
author_sort A. Setyan
collection DOAJ
description Regional new particle formation and growth events (NPEs) were observed on most days over the Sacramento and western Sierra foothills area of California in June 2010 during the Carbonaceous Aerosols and Radiative Effect Study (CARES). Simultaneous particle measurements at both the T0 (Sacramento, urban site) and the T1 (Cool, rural site located ~40 km northeast of Sacramento) sites of CARES indicate that the NPEs usually occurred in the morning with the appearance of an ultrafine mode at ~15 nm (in mobility diameter, <i>D</i><sub>m</sub>, measured by a mobility particle size spectrometer operating in the range 10-858 nm) followed by the growth of this modal diameter to ~50 nm in the afternoon. These events were generally associated with southwesterly winds bringing urban plumes from Sacramento to the T1 site. The growth rate was on average higher at T0 (7.1 ± 2.7 nm h<sup>−1</sup>) than at T1 (6.2 ± 2.5 nm h<sup>−1</sup>), likely due to stronger anthropogenic influences at T0. Using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), we investigated the evolution of the size-resolved chemical composition of new particles at T1. Our results indicate that the growth of new particles was driven primarily by the condensation of oxygenated organic species and, to a lesser extent, ammonium sulfate. New particles appear to be fully neutralized during growth, consistent with high NH<sub>3</sub> concentration in the region. Nitrogen-containing organic ions (i.e., CHN<sup>+</sup>, CH<sub>4</sub>N<sup>+</sup>, C<sub>2</sub>H<sub>3</sub>N<sup>+</sup>, and C<sub>2</sub>H<sub>4</sub>N<sup>+</sup>) that are indicative of the presence of alkyl-amine species in submicrometer particles enhanced significantly during the NPE days, suggesting that amines might have played a role in these events. Our results also indicate that the bulk composition of the ultrafine mode organics during NPEs was very similar to that of anthropogenically influenced secondary organic aerosol (SOA) observed in transported urban plumes. In addition, the concentrations of species representative of urban emissions (e.g., black carbon, CO, NO<sub>x</sub>, and toluene) were significantly higher whereas the photo-oxidation products of biogenic VOCs (volatile organic compounds) and the biogenically influenced SOA also increased moderately during the NPE days compared to the non-event days. These results indicate that the frequently occurring NPEs over the Sacramento and Sierra Nevada regions were mainly driven by urban plumes from Sacramento and the San Francisco Bay Area, and that the interaction of regional biogenic emissions with the urban plumes has enhanced the new particle growth. This finding has important implications for quantifying the climate impacts of NPEs on global scale.
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spelling doaj.art-fa3653c0ddda413b8edfa105ee5fb9602022-12-22T01:06:24ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242014-07-0114136477649410.5194/acp-14-6477-2014Chemistry of new particle growth in mixed urban and biogenic emissions – insights from CARESA. Setyan0C. Song1M. Merkel2W. B. Knighton3T. B. Onasch4M. R. Canagaratna5D. R. Worsnop6A. Wiedensohler7J. E. Shilling8Q. Zhang9Department of Environmental Toxicology, 1 Shields Ave., University of California, Davis, CA 95616, USAAtmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richmond, WA 99352, USALeibniz Institute for Tropospheric Research, 04318 Leipzig, GermanyMontana State University, Bozeman, MT 59717, USAAerodyne Research Inc., Billerica, MA 01821, USAAerodyne Research Inc., Billerica, MA 01821, USAAerodyne Research Inc., Billerica, MA 01821, USALeibniz Institute for Tropospheric Research, 04318 Leipzig, GermanyAtmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richmond, WA 99352, USADepartment of Environmental Toxicology, 1 Shields Ave., University of California, Davis, CA 95616, USARegional new particle formation and growth events (NPEs) were observed on most days over the Sacramento and western Sierra foothills area of California in June 2010 during the Carbonaceous Aerosols and Radiative Effect Study (CARES). Simultaneous particle measurements at both the T0 (Sacramento, urban site) and the T1 (Cool, rural site located ~40 km northeast of Sacramento) sites of CARES indicate that the NPEs usually occurred in the morning with the appearance of an ultrafine mode at ~15 nm (in mobility diameter, <i>D</i><sub>m</sub>, measured by a mobility particle size spectrometer operating in the range 10-858 nm) followed by the growth of this modal diameter to ~50 nm in the afternoon. These events were generally associated with southwesterly winds bringing urban plumes from Sacramento to the T1 site. The growth rate was on average higher at T0 (7.1 ± 2.7 nm h<sup>−1</sup>) than at T1 (6.2 ± 2.5 nm h<sup>−1</sup>), likely due to stronger anthropogenic influences at T0. Using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), we investigated the evolution of the size-resolved chemical composition of new particles at T1. Our results indicate that the growth of new particles was driven primarily by the condensation of oxygenated organic species and, to a lesser extent, ammonium sulfate. New particles appear to be fully neutralized during growth, consistent with high NH<sub>3</sub> concentration in the region. Nitrogen-containing organic ions (i.e., CHN<sup>+</sup>, CH<sub>4</sub>N<sup>+</sup>, C<sub>2</sub>H<sub>3</sub>N<sup>+</sup>, and C<sub>2</sub>H<sub>4</sub>N<sup>+</sup>) that are indicative of the presence of alkyl-amine species in submicrometer particles enhanced significantly during the NPE days, suggesting that amines might have played a role in these events. Our results also indicate that the bulk composition of the ultrafine mode organics during NPEs was very similar to that of anthropogenically influenced secondary organic aerosol (SOA) observed in transported urban plumes. In addition, the concentrations of species representative of urban emissions (e.g., black carbon, CO, NO<sub>x</sub>, and toluene) were significantly higher whereas the photo-oxidation products of biogenic VOCs (volatile organic compounds) and the biogenically influenced SOA also increased moderately during the NPE days compared to the non-event days. These results indicate that the frequently occurring NPEs over the Sacramento and Sierra Nevada regions were mainly driven by urban plumes from Sacramento and the San Francisco Bay Area, and that the interaction of regional biogenic emissions with the urban plumes has enhanced the new particle growth. This finding has important implications for quantifying the climate impacts of NPEs on global scale.http://www.atmos-chem-phys.net/14/6477/2014/acp-14-6477-2014.pdf
spellingShingle A. Setyan
C. Song
M. Merkel
W. B. Knighton
T. B. Onasch
M. R. Canagaratna
D. R. Worsnop
A. Wiedensohler
J. E. Shilling
Q. Zhang
Chemistry of new particle growth in mixed urban and biogenic emissions – insights from CARES
Atmospheric Chemistry and Physics
title Chemistry of new particle growth in mixed urban and biogenic emissions – insights from CARES
title_full Chemistry of new particle growth in mixed urban and biogenic emissions – insights from CARES
title_fullStr Chemistry of new particle growth in mixed urban and biogenic emissions – insights from CARES
title_full_unstemmed Chemistry of new particle growth in mixed urban and biogenic emissions – insights from CARES
title_short Chemistry of new particle growth in mixed urban and biogenic emissions – insights from CARES
title_sort chemistry of new particle growth in mixed urban and biogenic emissions insights from cares
url http://www.atmos-chem-phys.net/14/6477/2014/acp-14-6477-2014.pdf
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