skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Estimating Black Carbon Aging Time-Scales with a Particle-Resolved Aerosol Model

Abstract

Understanding the aging process of aerosol particles is important for assessing their chemical reactivity, cloud condensation nuclei activity, radiative properties and health impacts. In this study we investigate the aging of black carbon containing particles in an idealized urban plume using a new approach, the particleresolved aerosol model PartMC-MOSAIC. We present a method to estimate aging time-scales using an aging criterion based on cloud condensation nuclei activation. The results show a separation into a daytime regime where condensation dominates and a nighttime regime where coagulation dominates. For the chosen urban plume scenario, depending on the supersaturation threshold, the values for the aging timescales vary between 0.06 hours and 10 hours during the day, and between 6 hours and 20 hours during the night.

Authors:
; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
973702
Report Number(s):
PNNL-SA-64948
Journal ID: ISSN 0021-8502; JALSB7; TRN: US201006%%945
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Aerosol Science, (41):143-158; Journal Volume: 41
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; AEROSOLS; AGING; CARBON; CLOUDS; CONDENSATION NUCLEI; PLUMES; URBAN AREAS; TIME DEPENDENCE; ATMOSPHERIC CHEMISTRY

Citation Formats

Riemer, Nicole, West, Matt, Zaveri, Rahul A., and Easter, Richard C. Estimating Black Carbon Aging Time-Scales with a Particle-Resolved Aerosol Model. United States: N. p., 2010. Web. doi:10.1016/j.jaerosci.2009.08.009.
Riemer, Nicole, West, Matt, Zaveri, Rahul A., & Easter, Richard C. Estimating Black Carbon Aging Time-Scales with a Particle-Resolved Aerosol Model. United States. doi:10.1016/j.jaerosci.2009.08.009.
Riemer, Nicole, West, Matt, Zaveri, Rahul A., and Easter, Richard C. 2010. "Estimating Black Carbon Aging Time-Scales with a Particle-Resolved Aerosol Model". United States. doi:10.1016/j.jaerosci.2009.08.009.
@article{osti_973702,
title = {Estimating Black Carbon Aging Time-Scales with a Particle-Resolved Aerosol Model},
author = {Riemer, Nicole and West, Matt and Zaveri, Rahul A. and Easter, Richard C.},
abstractNote = {Understanding the aging process of aerosol particles is important for assessing their chemical reactivity, cloud condensation nuclei activity, radiative properties and health impacts. In this study we investigate the aging of black carbon containing particles in an idealized urban plume using a new approach, the particleresolved aerosol model PartMC-MOSAIC. We present a method to estimate aging time-scales using an aging criterion based on cloud condensation nuclei activation. The results show a separation into a daytime regime where condensation dominates and a nighttime regime where coagulation dominates. For the chosen urban plume scenario, depending on the supersaturation threshold, the values for the aging timescales vary between 0.06 hours and 10 hours during the day, and between 6 hours and 20 hours during the night.},
doi = {10.1016/j.jaerosci.2009.08.009},
journal = {Journal of Aerosol Science, (41):143-158},
number = ,
volume = 41,
place = {United States},
year = 2010,
month = 1
}
  • : A new two-dimensional aerosol bin scheme, which resolves both aerosol size and black carbon (BC) mixing state for BC aging processes (e.g., condensation and coagulation), has been developed and implemented into the WRF-chem model (MS-resolved WRF-chem). The mixing state of BC simulated by this model is compared with direct measurements over the East Asian region in spring 2009. Model simulations generally reproduce the observed features of the BC mixing state, such as the size-dependent number fractions of BC-containing and BC-free particles and the coating thickness of BC-containing particles. Sensitivity simulations show that the condensation process is dominant for themore » growth of thinly coated BC particles, while the coagulation process is necessary to produce thickly coated BC particles. Off-line optical and radiative calculations assuming an average mixing state for each size bin show that the domain- and period-averaged absorption coefficient and heating rate by aerosols are overestimated by 30 – 40% in the boundary layer compared with a benchmark simulation with the detailed treatment of mixing state. The absolute value of aerosol radiative forcing is also overestimated (10%, 3 W m-2) at the surface. However, these overestimations are reduced considerably when all the parameters (including mass and number concentration) are calculated with the simple treatment of mixing state. This is because the overestimation of radiative parameters due to higher absorption efficiency (compared with the benchmark simulation) is largely canceled by the underestimation of BC concentrations due to efficient wet removal processes. The overall errors in radiative forcing can be much smaller because of this cancellation but for the wrong reasons.« less
  • An automated Time Resolved Aerosol Collector (TRAC) has been developed for sequential sampling of field-collected aerosols for laboratory-based Computer Controlled Scanning Electron Microscopy/Energy Dispersed X-ray (CCSEM/EDX) single particle analysis. The collector is optimized for use of grid-supported 20 nm carbon films as deposition substrates. The carbon films have low enough X-ray background to permit EDX analysis down to 0.1-0.2 ?m particles, including detection of low-Z elements: C, N, & O. The TRAC provides unattended sampling onto a set of 151 individual grids, at sequential time intervals as short as 1 min. After collection, the samples are sealed and refrigerated pendingmore » analysis. The utility of the TRAC-CCSEM/EDX approach is exemplified using the aerosol samples collected during the Texas 2000 Air Quality Studies (Aug. 15 ? Sept. 15, 2000). We are able to quantitatively follow the time evolution in the relative contribution of non-volatile particles such as ammonium sulfate, mineral dust, sea salt, carbonaceous, etc. in the aerosol make up. The results show, among other things, the diurnal cycles in appearance of fine carbonaceous & ammonium sulfate particles & substantial mixing/coating of mineral particles with ammonium sulfates.« less
  • The soot-particle aerosol mass spectrometer (SP-AMS) uses an intra-cavity infrared laser to vaporize refractory black carbon (rBC) containing particles, making the particle beam–laser beam overlap critical in determining the collection efficiency (CE) for rBC and associated non-refractory particulate matter (NR-PM). This work evaluates the ability of the SP-AMS to quantify rBC and NR-PM mass in internally mixed particles with different thicknesses of organic coating. Using apparent relative ionization efficiencies for uncoated and thickly coated rBC particles, we report measurements of SP-AMS sensitivity to NR-PM and rBC, for Regal Black, the recommended particulate calibration material. Beam width probe (BWP) measurements aremore » used to illustrate an increase in sensitivity for highly coated particles due to narrowing of the particle beam, which enhances the CE of the SP-AMS by increasing the laser beam–particle beam overlap. Assuming complete overlap for thick coatings, we estimate CE for bare Regal Black particles of 0.6 ± 0.1, which suggests that previously measured SP-AMS sensitivities to Regal Black were underestimated by up to a factor of 2. The efficacy of the BWP measurements is highlighted by studies at a busy road in downtown Toronto and at a non-roadside location, which show particle beam widths similar to, but greater than that of bare Regal Black and coated Regal Black, respectively. Further BWP measurements at field locations will help to constrain the range of CE for fresh and aged rBC-containing particles. The ability of the SP-AMS to quantitatively assess the composition of internally mixed particles is validated through measurements of laboratory-generated organic coated particles, which demonstrate that the SP-AMS can quantify rBC and NR-PM over a wide range of particle compositions and rBC core sizes.« less
    Cited by 17
  • The mixing state of soot particles in the atmosphere is of crucial importance for assessing their climatic impact, since it governs their chemical reactivity, cloud condensation nuclei activity and radiative properties. To improve the mixing state representation in models, we present a new approach, the stochastic particle-resolved model PartMC-MOSAIC, which explicitly resolves the composition of individual particles in a given population of different types of aerosol particles. This approach accurately tracks the evolution of the mixing state of particles due to emission, dilution, condensation and coagulation. To make this direct stochastic particle-based method practical, we implemented a new multiscale stochasticmore » coagulation method. With this method we achieved optimal efficiency for applications when the coagulation kernel is highly non-uniform, as is the case for many realistic applications. PartMC-MOSAIC was applied to an idealized urban plume case representative of a large urban area to simulate the evolution of carbonaceous aerosols of different types due to coagulation and condensation. For this urban plume scenario we quantified the individual processes that contribute to the aging of the aerosol distribution, illustrating the capabilities of our modeling approach. The results showed for the first time the multidimensional structure of particle composition, which is usually lost in internally-mixed sectional or modal aerosol models.« less