Identification

Title

Cloud activating properties of aerosol observed during CELTIC

Abstract

Measurements of aerosol size distribution, chemical composition, and cloud condensation nuclei (CCN) concentration were performed during the Chemical Emission, Loss, Transformation, and Interactions with Canopies (CELTIC) field program at Duke Forest in North Carolina. A kinetic model of the cloud activation of ambient aerosol in the chamber of the CCN instrument was used to perform an aerosol-CCN closure study. This study advances prior investigations by employing a novel fitting algorithm that was used to integrate scanning mobility particle sizer (SMPS) measurements of aerosol number size distribution and aerosol mass spectrometer (AMS) measurements of the mass size distribution for sulfate, nitrate, ammonium, and organics into a single, coherent description of the ambient aerosol in the size range critical to aerosol activation (around 100-nm diameter). Three lognormal aerosol size modes, each with a unique internally mixed composition, were used as input into the kinetic model. For the two smaller size modes, which control CCN number concentration, organic aerosol mass fractions for the defined cases were between 58% and 77%. This study is also unique in that the water vapor accommodation coefficient was estimated based on comparing the initial timing for CCN activation in the instrument chamber with the activation predicted by the kinetic model. The kinetic model overestimated measured CCN concentrations, especially under polluted conditions. Prior studies have attributed a positive model bias to an incomplete understanding of the aerosol composition, especially the role of organics in the activation process. This study shows that including measured organic mass fractions with an assumed organic aerosol speciation profile (pinic acid, fulvic acid, and levoglucosan) and an assumed organic aerosol solubility of 0.02 kg kg⁻¹ still resulted in a significant model positive bias for polluted case study periods. The slope and y intercept for the CCN predicted versus CCN observed regression was found to be 1.9 and -180 cm⁻³, respectively. The overprediction generally does not exceed uncertainty limits but is indicative that a bias exists in the measurements or application of model. From this study, uncertainties in the particle number and mass size distributions as the cause for the model bias can be ruled out. The authors are also confident that the model is including the effects of growth kinetics on predicted activated number. However, one cannot rule out uncertainties associated with poorly characterized CCN measurement biases, uncertainties in assumed organic solubility, and uncertainties in aerosol mixing state. Sensitivity simulations suggest that assuming either an insoluble organic fraction or external aerosol mixing were both sufficient to reconcile the model bias.

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document

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http://n2t.net/ark:/85065/d7xd11xj

codeSpace

Dataset language

eng

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geoscientificInformation

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title

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publication

effective date

2016-01-01T00:00:00Z

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publication

effective date

2007-02-01T00:00:00Z

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Copyright 2007 American Meteorological Society (AMS). Permission to use figures, tables, and brief excerpts from this work in scientific and educational works is hereby granted provided that the source is acknowledged. Any use of material in this work that is determined to be "fair use" under Section 107 or that satisfies the conditions specified in Section 108 of the U.S. Copyright Law (17 USC, as revised by P.L. 94-553) does not require the Society's permission. Republication, systematic reproduction, posting in electronic form on servers, or other uses of this material, except as exempted by the above statements, requires written permission or license from the AMS. Additional details are provided in the AMS Copyright Policies, available from the AMS at 617-227-2425 or amspubs@ametsoc.org. Permission to place a copy of this work on this server has been provided by the AMS. The AMS does not guarantee that the copy provided here is an accurate copy of the published work.

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OpenSky Support

organisation name

UCAR/NCAR - Library

full postal address

PO Box 3000

Boulder

80307-3000

email address

opensky@ucar.edu

web address

http://opensky.ucar.edu/

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pointOfContact

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