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Title: Global 2-D intercomparison of sectional and modal aerosol modules

Abstract

We present an intercomparison of two aerosol modules, one sectional, one modal, in a global 2-D model in order to differentiate their behavior for tropospheric and stratospheric applications. We model only binary sulfuric acid-water aerosols in this study. Two versions of the sec-tional model and three versions of the modal model are used to test the sensitivity of background aerosol mass and size distribution to the number of bins or modes and to the pre-scribed width of the largest mode. We find modest sensitivity to the number of bins (40 vs 150) used in the sectional model. Aerosol mass is found to be reduced in a modal model if care is not taken in selecting the width of the largest lognormal mode, reflecting differences in sedimentation in the middle stratosphere. The size distributions calculated by the sec-tional model can be better matched by a modal model with four modes rather than three modes in most but not all sit-uations. A simulation of aerosol decay following the 1991 eruption of Mt. Pinatubo shows that the representation of the size distribution can have a signflcant impact on model-calculated aerosol decay rates in the stratosphere. Between 1991 and 1995, aerosol mass and surfacemore » area density calcu-lated by two versions of the modal model adequately match results from the sectional model. Calculated effective radius for the same time period shows more intermodel variability.« less

Authors:
; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
908733
Report Number(s):
PNWD-SA-7668
TRN: US200722%%765
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Atmospheric Chemistry and Physics, 7(9):2339-2355; Journal Volume: 7; Journal Issue: 9
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; AEROSOLS; TWO-DIMENSIONAL CALCULATIONS; MATHEMATICAL MODELS; STRATOSPHERE; COMPARATIVE EVALUATIONS; TROPOSPHERE; SULFURIC ACID; WATER VAPOR

Citation Formats

Weisenstein, D K, Penner, J E, Herzog, M, and Liu, Xiaohong. Global 2-D intercomparison of sectional and modal aerosol modules. United States: N. p., 2007. Web. doi:10.5194/acp-7-2339-2007.
Weisenstein, D K, Penner, J E, Herzog, M, & Liu, Xiaohong. Global 2-D intercomparison of sectional and modal aerosol modules. United States. doi:10.5194/acp-7-2339-2007.
Weisenstein, D K, Penner, J E, Herzog, M, and Liu, Xiaohong. Tue . "Global 2-D intercomparison of sectional and modal aerosol modules". United States. doi:10.5194/acp-7-2339-2007.
@article{osti_908733,
title = {Global 2-D intercomparison of sectional and modal aerosol modules},
author = {Weisenstein, D K and Penner, J E and Herzog, M and Liu, Xiaohong},
abstractNote = {We present an intercomparison of two aerosol modules, one sectional, one modal, in a global 2-D model in order to differentiate their behavior for tropospheric and stratospheric applications. We model only binary sulfuric acid-water aerosols in this study. Two versions of the sec-tional model and three versions of the modal model are used to test the sensitivity of background aerosol mass and size distribution to the number of bins or modes and to the pre-scribed width of the largest mode. We find modest sensitivity to the number of bins (40 vs 150) used in the sectional model. Aerosol mass is found to be reduced in a modal model if care is not taken in selecting the width of the largest lognormal mode, reflecting differences in sedimentation in the middle stratosphere. The size distributions calculated by the sec-tional model can be better matched by a modal model with four modes rather than three modes in most but not all sit-uations. A simulation of aerosol decay following the 1991 eruption of Mt. Pinatubo shows that the representation of the size distribution can have a signflcant impact on model-calculated aerosol decay rates in the stratosphere. Between 1991 and 1995, aerosol mass and surface area density calcu-lated by two versions of the modal model adequately match results from the sectional model. Calculated effective radius for the same time period shows more intermodel variability.},
doi = {10.5194/acp-7-2339-2007},
journal = {Atmospheric Chemistry and Physics, 7(9):2339-2355},
number = 9,
volume = 7,
place = {United States},
year = {Tue May 08 00:00:00 EDT 2007},
month = {Tue May 08 00:00:00 EDT 2007}
}
  • Many of the next generation of global climate models will include aerosol schemes which explicitly simulate the microphysical processes that determine the particle size distribution. These models enable aerosol optical properties and cloud condensation nuclei (CCN) concentrations to be determined by fundamental aerosol processes, which should lead to a more physically based simulation of aerosol direct and indirect radiative forcings. This study examines the global variation in particle size distribution simulated by twelve global aerosol microphysics models to quantify model diversity and to identify any common biases against observations. Evaluation against size distribution measurements from a new European network ofmore » aerosol supersites shows that the mean model agrees quite well with the observations at many sites on the annual mean, but there are some seasonal biases common to many sites. In particular, at many of these European sites, the accumulation mode number concentration is biased low during winter and Aitken mode concentrations tend to be overestimated in winter and underestimated in summer. At high northern latitudes, the models strongly underpredict Aitken and accumulation particle concentrations compared to the measurements, consistent with previous studies that have highlighted the poor performance of global aerosol models in the Arctic. In the marine boundary layer, the models capture the observed meridional variation in the size distribution, which is dominated by the Aitken mode at high latitudes, with an increasing concentration of accumulation particles with decreasing latitude. Considering vertical profiles, the models reproduce the observed peak in total particle concentrations in the upper troposphere due to new particle formation, although modelled peak concentrations tend to be biased high over Europe. Overall, the results suggest that most global aerosol microphysics models simulate the global variation of the particle size distribution with a good degree of skill, but some models are in poor agreement with the observations. Further work is required to better constrain size-resolved primary and secondary particle number sources, and an improved understanding of nucleation and growth (e.g. the role of nitrate and secondary organics) will improve the fidelity of simulated particle size distributions.« less
  • This paper evaluates the current status of global modeling of the organic aerosol (OA) in the troposphere and analyzes the differences between models as well as between models and observations. Thirty-one global chemistry transport models (CTMs) and general circulation models (GCMs) have participated in this intercomparison, in the framework of AeroCom phase II. The simulation of OA varies greatly between models in terms of the magnitude of primary emissions, secondary OA (SOA) formation, the number of OA species used (2 to 62), the complexity of OA parameterizations (gas-particle partitioning, chemical aging, multiphase chemistry, aerosol microphysics), and the OA physical, chemicalmore » and optical properties. The diversity of the global OA simulation results has increased since earlier AeroCom experiments, mainly due to the increasing complexity of the SOA parameterization in models, and the implementation of new, highly uncertain, OA sources. Diversity of over one order of magnitude exists in the modeled vertical distribution of OA concentrations that deserves a dedicated future study. Furthermore, although the OA / OC ratio depends on OA sources and atmospheric processing, and is important for model evaluation against OA and OC observations, it is resolved only by a few global models. The median global primary OA (POA) source strength is 56 Tg a –1 (range 34–144 Tg a −1) and the median SOA source strength (natural and anthropogenic) is 19 Tg a –1 (range 13–121 Tg a −1). Among the models that take into account the semi-volatile SOA nature, the median source is calculated to be 51 Tg a –1 (range 16–121 Tg a −1), much larger than the median value of the models that calculate SOA in a more simplistic way (19 Tg a –1; range 13–20 Tg a –1, with one model at 37 Tg a −1). The median atmospheric burden of OA is 1.4 Tg (24 models in the range of 0.6–2.0 Tg and 4 between 2.0 and 3.8 Tg), with a median OA lifetime of 5.4 days (range 3.8–9.6 days). In models that reported both OA and sulfate burdens, the median value of the OA/sulfate burden ratio is calculated to be 0.77; 13 models calculate a ratio lower than 1, and 9 models higher than 1. For 26 models that reported OA deposition fluxes, the median wet removal is 70 Tg a –1 (range 28–209 Tg a −1), which is on average 85% of the total OA deposition. Fine aerosol organic carbon (OC) and OA observations from continuous monitoring networks and individual field campaigns have been used for model evaluation. At urban locations, the model–observation comparison indicates missing knowledge on anthropogenic OA sources, both strength and seasonality. The combined model–measurements analysis suggests the existence of increased OA levels during summer due to biogenic SOA formation over large areas of the USA that can be of the same order of magnitude as the POA, even at urban locations, and contribute to the measured urban seasonal pattern. Global models are able to simulate the high secondary character of OA observed in the atmosphere as a result of SOA formation and POA aging, although the amount of OA present in the atmosphere remains largely underestimated, with a mean normalized bias (MNB) equal to –0.62 (–0.51) based on the comparison against OC (OA) urban data of all models at the surface, –0.15 (+0.51) when compared with remote measurements, and –0.30 for marine locations with OC data. The mean temporal correlations across all stations are low when compared with OC (OA) measurements: 0.47 (0.52) for urban stations, 0.39 (0.37) for remote stations, and 0.25 for marine stations with OC data. The combination of high (negative) MNB and higher correlation at urban stations when compared with the low MNB and lower correlation at remote sites suggests that knowledge about the processes that govern aerosol processing, transport and removal, on top of their sources, is important at the remote stations. There is no clear change in model skill with increasing model complexity with regard to OC or OA mass concentration. As a result, the complexity is needed in models in order to distinguish between anthropogenic and natural OA as needed for climate mitigation, and to calculate the impact of OA on climate accurately.« less
  • The AeroCom exercise diagnoses multi-component aerosol modules in global modeling. In an initial assessment global fields for mass and for mid-visible aerosol optical thickness (aot) were compared among aerosol component modules of 21 different global models. There is general agreement among models for the annual global mean of component combined aot. At 0.12 to 0.14, simulated aot values are at the lower end of global averages suggested by remote sensing from ground (AERONET ca 0.14) and space (MODIS-MISR composite ca 0.16). More detailed comparisons, however, reveal that larger differences in regional distribution and significant differences in compositional mixture have remained.more » Of particular concern is the large model diversity for contributions by dust and carbon, because it leads to significant uncertainty in aerosol absorption (aab). Since not only aot but also aab influence the aerosol impact on the radiative energy-balance, aerosol (direct) forcing uncertainty in modeling is larger than differences in aot might suggest. New diagnostic approaches are proposed to trace model differences in terms of aerosol processing and transport: These include the prescription of common input (e.g. amount, size and injection of aerosol component emissions) and the use of observational capabilities from ground (e.g. measurements networks) and space (e.g. correlations between retrieved aerosol and cloud properties).« less
  • The dynamics of aerosols in the marine boundary layer (MBL) are simulated with the marine boundary layer aerosol model (MARBLES), a one-dimensional, multicomponent sectional aerosol model [{ital Fitzgerald} {ital et al.}, this issue; {ital Gelbard} {ital et al.}, this issue]. First, to illustrate how the various aerosol processes influence the particle size distribution, the model was run with one or two processes operating on the same initial size distribution. Because of current interest in the effects of cloud processing of aerosols and exchange of aerosols with the free troposphere (FT) on marine aerosol size distributions, these two processes are examinedmore » in considerable detail. The simulations show that the effect of cloud processing (characteristic double-peaked size distribution) in the upper part of the MBL is manifested at the surface on a timescale that is much faster than changes due to exchange with the FT, assuming a typical exchange velocity of 0.6 cmthinsps{sup {minus}1}. The model predicts that the FT can be a significant source of particles for the MBL in the size range of the cloud-processing minimum, between the unactivated interstitial particles and the cloud condensation nuclei (CCN) which have grown as a result of conversion of dissolved SO{sub 2} to sulfate in cloud droplets. The model was also used to simulate the evolution of the aerosol size distribution in an air mass advecting from the east coast of the United States out over the ocean for up to 10 days. The modification of a continental aerosol size distribution to one that is remote marine in character occurs on a timescale of 6{endash}8 days. Nucleation was not observed in the base case 10-day advection simulation which assumed rather typical meteorological conditions. However, significant nucleation was predicted under a more favorable (albeit, atypical) combination of conditions which included significant precipitation scavenging (5 mmthinsph{sup {minus}1} of rain for 12 hours), colder temperatures by 10thinsp{degree}C (283 K at the surface decreasing to 278 K at 1000 m) and a high DMS flux (40 {mu}molthinspm{sup {minus}2}thinspd{sup {minus}1}). In a test of model self initialization, long-term (8{endash}10 days) predictions of marine aerosol size distributions were found to be essentially independent of initial conditions. {copyright} 1998 American Geophysical Union« less
  • An airborne continuous wave (CW) focused CO{sub 2} Doppler lidar and a ground-based pulsed CO{sub 2} Doppler lidar were used to obtain seven pairs of comparative measurements of tropospheric aerosol backscatter profiles at 10.6 {mu}m wavelength, near Denver, Colorado, during a 20-day period in July 1982. In regions of uniform backscatter the two lidars show good agreement, with differences usually less than {approximately}50% near 8-km altitude and less than a factor of 2 or 3 elsewhere but with the pulsed lidar often lower than the CW lidar. Near sharp backscatter gradients the two lidars show poorer agreement, with the pulsedmore » lidar usually higher than the CW lidar. Most discrepancies arise from a combination of atmospheric factors and instrument factors, particularly small-scale areal and temporal backscatter heterogeneity above the planetary boundary layer, unusual large-scale vertical backscatter structure in the upper troposphere and lower stratosphere, and differences in the spatial resolution, detection threshold, and noise estimation for the two lidars.« less