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  • 1
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    Online Resource
    Chemical transport models often underestimate inorganic aerosol acidity in remote regions of the atmosphere
    Springer Science and Business Media LLC ; 2021
    In:  Communications Earth & Environment Vol. 2, No. 1 ( 2021-05-14)
    Details
    In: Communications Earth & Environment, Springer Science and Business Media LLC, Vol. 2, No. 1 ( 2021-05-14)
    Abstract: The inorganic fraction of fine particles affects numerous physicochemical processes in the atmosphere. However, there is large uncertainty in its burden and composition due to limited global measurements. Here, we present observations from eleven different aircraft campaigns from around the globe and investigate how aerosol pH and ammonium balance change from polluted to remote regions, such as over the oceans. Both parameters show increasing acidity with remoteness, at all altitudes, with pH decreasing from about 3 to about −1 and ammonium balance decreasing from almost 1 to nearly 0. We compare these observations against nine widely used chemical transport models and find that the simulations show more scatter (generally R 2   〈  0.50) and typically predict less acidic aerosol in the most remote regions. These differences in observations and predictions are likely to result in underestimating the model-predicted direct radiative cooling effect for sulfate, nitrate, and ammonium aerosol by 15–39%.
    Type of Medium: Online Resource
    ISSN: 2662-4435
    URL: Article
    DOI: 10.1038/s43247-021-00164-0
    Language: English
    Publisher: Springer Science and Business Media LLC
    Publication Date: 2021
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  • 2
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    Chemical Characterization of Aerosols on the East Coast of the United States Using Aircraft and Ground-Based Stations during the CLAMS Experiment
    American Meteorological Society ; 2005
    In:  Journal of the Atmospheric Sciences Vol. 62, No. 4 ( 2005-04-01), p. 934-946
    Details
    In: Journal of the Atmospheric Sciences, American Meteorological Society, Vol. 62, No. 4 ( 2005-04-01), p. 934-946
    Abstract: The Chesapeake Lighthouse and Aircraft Measurements for Satellites (CLAMS) experiment was carried out off the central East Coast of the United States in July 2001. During CLAMS, aerosol particle mass was measured at two ground stations and on the University of Washington’s Convair 580 research aircraft. Physical and chemical characteristics of the aerosols were identified and quantified. Three main aerosol regimes were identified in the region and are discussed in this work: local pollution/sea salt background, long-range transported dust, and long-range transported pollution. The major component measured in the fine mode of the aerosol on the ground at Wallops Island, Virginia, was sulfate, estimated as NH4HSO4, which accounted for 55% ± 9% on average of the fine particle mass (FPM) during the experiment period. Black carbon concentrations accounted for 3% ± 1% of FPM; soil dust was also present, representing on average 6% ± 8% of FPM. The difference between the sum of the masses of the measured compounds and the total fine particle mass was 36% ± 10% of FPM, which is attributed primarily to nitrates and organic carbon that were not measured. Aerosol chemical composition in the atmospheric column is also discussed and compared with ground-based measurements. Aerosol dust concentration reached 40% of FPM during an incursion of Saharan dust between 24 and 26 July. Sulfate aerosol reached 70% of FPM during the transport of regional pollution on 17 July. Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol optical thickness, coupled with air parcel back trajectories, supported the conclusion of episodes of long-range transport of dust from the Sahara Desert and pollutants from the continental United States.
    Type of Medium: Online Resource
    ISSN: 1520-0469 , 0022-4928
    URL: Article
    DOI: 10.1175/JAS3388.1
    RVK:
    UA 4800
    Language: English
    Publisher: American Meteorological Society
    Publication Date: 2005
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  • 3
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    The response of the Amazon ecosystem to the photosynthetically active radiation fields: integrating impacts of biomass burning aerosol and clouds in the NASA GEOS Earth system model
    Copernicus GmbH ; 2021
    In:  Atmospheric Chemistry and Physics Vol. 21, No. 18 ( 2021-09-24), p. 14177-14197
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 18 ( 2021-09-24), p. 14177-14197
    Abstract: Abstract. The Amazon experiences fires every year, and the resulting biomass burning aerosols, together with cloud particles, influence the penetration of sunlight through the atmosphere, increasing the ratio of diffuse to direct photosynthetically active radiation (PAR) reaching the vegetation canopy and thereby potentially increasing ecosystem productivity. In this study, we use the NASA Goddard Earth Observing System (GEOS) model with coupled aerosol, cloud, radiation, and ecosystem modules to investigate the impact of Amazon biomass burning aerosols on ecosystem productivity, as well as the role of the Amazon's clouds in tempering this impact. The study focuses on a 7-year period (2010–2016) during which the Amazon experienced a variety of dynamic environments (e.g., La Niña, normal years, and El Niño). The direct radiative impact of biomass burning aerosols on ecosystem productivity – called here the aerosol diffuse radiation fertilization effect – is found to increase Amazonian gross primary production (GPP) by 2.6 % via a 3.8 % increase in diffuse PAR (DFPAR) despite a 5.4 % decrease in direct PAR (DRPAR) on multiyear average during burning seasons. On a monthly basis, this increase in GPP can be as large as 9.9 % (occurring in August 2010). Consequently, the net primary production (NPP) in the Amazon is increased by 1.5 %, or ∼92 Tg C yr−1 – equivalent to ∼37 % of the average carbon lost due to Amazon fires over the 7 years considered. Clouds, however, strongly regulate the effectiveness of the aerosol diffuse radiation fertilization effect. The efficiency of this fertilization effect is the highest in cloud-free conditions and linearly decreases with increasing cloud amount until the cloud fraction reaches ∼0.8, at which point the aerosol-influenced light changes from being a stimulator to an inhibitor of plant growth. Nevertheless, interannual changes in the overall strength of the aerosol diffuse radiation fertilization effect are primarily controlled by the large interannual changes in biomass burning aerosols rather than by changes in cloudiness during the studied period.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-21-14177-2021
    DOI: 10.5194/acp-21-14177-2021-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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  • 4
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    Planning, implementation, and first results of the Tropical Composition, Cloud and Climate Coupling Experiment (TC4)
    American Geophysical Union (AGU) ; 2010
    In:  Journal of Geophysical Research Vol. 115 ( 2010-07-15)
    Details
    In: Journal of Geophysical Research, American Geophysical Union (AGU), Vol. 115 ( 2010-07-15)
    Type of Medium: Online Resource
    ISSN: 0148-0227
    URL: Article
    DOI: 10.1029/2009JD013073
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2010
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  • 5
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    Status and future of numerical atmospheric aerosol prediction with a focus on data requirements
    Copernicus GmbH ; 2018
    In:  Atmospheric Chemistry and Physics Vol. 18, No. 14 ( 2018-07-25), p. 10615-10643
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 14 ( 2018-07-25), p. 10615-10643
    Abstract: Abstract. Numerical prediction of aerosol particle properties has become an important activity at many research and operational weather centers. This development is due to growing interest from a diverse set of stakeholders, such as air quality regulatory bodies, aviation and military authorities, solar energy plant managers, climate services providers, and health professionals. Owing to the complexity of atmospheric aerosol processes and their sensitivity to the underlying meteorological conditions, the prediction of aerosol particle concentrations and properties in the numerical weather prediction (NWP) framework faces a number of challenges. The modeling of numerous aerosol-related parameters increases computational expense. Errors in aerosol prediction concern all processes involved in the aerosol life cycle including (a) errors on the source terms (for both anthropogenic and natural emissions), (b) errors directly dependent on the meteorology (e.g., mixing, transport, scavenging by precipitation), and (c) errors related to aerosol chemistry (e.g., nucleation, gas–aerosol partitioning, chemical transformation and growth, hygroscopicity). Finally, there are fundamental uncertainties and significant processing overhead in the diverse observations used for verification and assimilation within these systems. Indeed, a significant component of aerosol forecast development consists in streamlining aerosol-related observations and reducing the most important errors through model development and data assimilation. Aerosol particle observations from satellite- and ground-based platforms have been crucial to guide model development of the recent years and have been made more readily available for model evaluation and assimilation. However, for the sustainability of the aerosol particle prediction activities around the globe, it is crucial that quality aerosol observations continue to be made available from different platforms (space, near surface, and aircraft) and freely shared. This paper reviews current requirements for aerosol observations in the context of the operational activities carried out at various global and regional centers. While some of the requirements are equally applicable to aerosol–climate, the focus here is on global operational prediction of aerosol properties such as mass concentrations and optical parameters. It is also recognized that the term “requirements” is loosely used here given the diversity in global aerosol observing systems and that utilized data are typically not from operational sources. Most operational models are based on bulk schemes that do not predict the size distribution of the aerosol particles. Others are based on a mix of “bin” and bulk schemes with limited capability of simulating the size information. However the next generation of aerosol operational models will output both mass and number density concentration to provide a more complete description of the aerosol population. A brief overview of the state of the art is provided with an introduction on the importance of aerosol prediction activities. The criteria on which the requirements for aerosol observations are based are also outlined. Assimilation and evaluation aspects are discussed from the perspective of the user requirements.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-18-10615-2018
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
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  • 6
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    Change in Tropospheric Ozone in the Recent Decades and Its Contribution to Global Total Ozone
    American Geophysical Union (AGU) ; 2022
    In:  Journal of Geophysical Research: Atmospheres Vol. 127, No. 22 ( 2022-11-27)
    Details
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 127, No. 22 ( 2022-11-27)
    Abstract: Global total column ozone increased about 4 DU from 2005 to 2018 and about 60% of this increase due to tropospheric ozone Tropospheric ozone increases depend primarily on increased regional emissions of ozone precursors, for example, volatile organic compounds The Goddard Earth observing system chemistry climate model underestimates the observed tropospheric ozone increase, as a result of underestimated NO 2 emissions increase
    Type of Medium: Online Resource
    ISSN: 2169-897X , 2169-8996
    URL: Article
    DOI: 10.1029/2022JD037170
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2022
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  • 7
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    Development of an Ozone Monitoring Instrument (OMI) aerosol index (AI) data assimilation scheme for aerosol modeling over bright surfaces – a step toward direct radiance assimilation in the UV spectrum
    Copernicus GmbH ; 2021
    In:  Geoscientific Model Development Vol. 14, No. 1 ( 2021-01-05), p. 27-42
    Details
    In: Geoscientific Model Development, Copernicus GmbH, Vol. 14, No. 1 ( 2021-01-05), p. 27-42
    Abstract: Abstract. Using the Vector LInearized Discrete Ordinate Radiative Transfer (VLIDORT) code as the main driver for forward model simulations, a first-of-its-kind data assimilation scheme has been developed for assimilating Ozone Monitoring Instrument (OMI) aerosol index (AI) measurements into the Naval Aerosol Analysis and Predictive System (NAAPS). This study suggests that both root mean square error (RMSE) and absolute errors can be significantly reduced in NAAPS analyses with the use of OMI AI data assimilation when compared to values from NAAPS natural runs. Improvements in model simulations demonstrate the utility of OMI AI data assimilation for aerosol model analysis over cloudy regions and bright surfaces. However, the OMI AI data assimilation alone does not outperform aerosol data assimilation that uses passive-based aerosol optical depth (AOD) products over cloud-free skies and dark surfaces. Further, as AI assimilation requires the deployment of a fully multiple-scatter-aware radiative transfer model in the forward simulations, computational burden is an issue. Nevertheless, the newly developed modeling system contains the necessary ingredients for assimilation of radiances in the ultraviolet (UV) spectrum, and our study shows the potential of direct radiance assimilation at both UV and visible spectrums, possibly coupled with AOD assimilation, for aerosol applications in the future. Additional data streams can be added, including data from the TROPOspheric Monitoring Instrument (TROPOMI), the Ozone Mapping and Profiler Suite (OMPS), and eventually the Plankton, Aerosol, Cloud and ocean Ecosystem (PACE) mission.
    Type of Medium: Online Resource
    ISSN: 1991-9603
    URL: Article
    URL: Article
    DOI: 10.5194/gmd-14-27-2021
    DOI: 10.5194/gmd-14-27-2021-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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  • 8
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    Current state of the global operational aerosol multi‐model ensemble: An update from the International Cooperative for Aerosol Prediction (ICAP)
    Wiley ; 2019
    In:  Quarterly Journal of the Royal Meteorological Society Vol. 145, No. S1 ( 2019-09), p. 176-209
    Details
    In: Quarterly Journal of the Royal Meteorological Society, Wiley, Vol. 145, No. S1 ( 2019-09), p. 176-209
    Abstract: Since the first International Cooperative for Aerosol Prediction (ICAP) multi‐model ensemble (MME) study, the number of ICAP global operational aerosol models has increased from five to nine. An update of the current ICAP status is provided, along with an evaluation of the performance of ICAP‐MME over 2012–2017, with a focus on June 2016–May 2017. Evaluated with ground‐based Aerosol Robotic Network (AERONET) aerosol optical depth (AOD) and data assimilation quality MODerate‐resolution Imaging Spectroradiometer (MODIS) retrieval products, the ICAP‐MME AOD consensus remains the overall top‐scoring and most consistent performer among all models in terms of root‐mean‐square error (RMSE), bias and correlation for total, fine‐ and coarse‐mode AODs as well as dust AOD; this is similar to the first ICAP‐MME study. Further, over the years, the performance of ICAP‐MME is relatively stable and reliable compared to more variability in the individual models. The extent to which the AOD forecast error of ICAP‐MME can be predicted is also examined. Leading predictors are found to be the consensus mean and spread. Regression models of absolute forecast errors were built for AOD forecasts of different lengths for potential applications. ICAP‐MME performance in terms of modal AOD RMSEs of the 21 regionally representative sites over 2012–2017 suggests a general tendency for model improvements in fine‐mode AOD, especially over Asia. No significant improvement in coarse‐mode AOD is found overall for this time period.
    Type of Medium: Online Resource
    ISSN: 0035-9009 , 1477-870X
    URL: Issue
    URL: Article
    DOI: 10.1002/qj.v145.S1
    DOI: 10.1002/qj.3497
    RVK:
    UA 1000
    RVK:
    UA 7650
    Language: English
    Publisher: Wiley
    Publication Date: 2019
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  • 9
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    Characterization of organic aerosol across the global remote troposphere: a comparison of ATom measurements and global chemistry models
    Copernicus GmbH ; 2020
    In:  Atmospheric Chemistry and Physics Vol. 20, No. 8 ( 2020-04-21), p. 4607-4635
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 8 ( 2020-04-21), p. 4607-4635
    Abstract: Abstract. The spatial distribution and properties of submicron organic aerosol (OA) are among the key sources of uncertainty in our understanding of aerosol effects on climate. Uncertainties are particularly large over remote regions of the free troposphere and Southern Ocean, where very few data have been available and where OA predictions from AeroCom Phase II global models span 2 to 3 orders of magnitude, greatly exceeding the model spread over source regions. The (nearly) pole-to-pole vertical distribution of non-refractory aerosols was measured with an aerosol mass spectrometer onboard the NASA DC-8 aircraft as part of the Atmospheric Tomography (ATom) mission during the Northern Hemisphere summer (August 2016) and winter (February 2017). This study presents the first extensive characterization of OA mass concentrations and their level of oxidation in the remote atmosphere. OA and sulfate are the major contributors by mass to submicron aerosols in the remote troposphere, together with sea salt in the marine boundary layer. Sulfate was dominant in the lower stratosphere. OA concentrations have a strong seasonal and zonal variability, with the highest levels measured in the lower troposphere in the summer and over the regions influenced by biomass burning from Africa (up to 10 µg sm−3). Lower concentrations (∼0.1–0.3 µg sm−3) are observed in the northern middle and high latitudes and very low concentrations (〈0.1 µg sm−3) in the southern middle and high latitudes. The ATom dataset is used to evaluate predictions of eight current global chemistry models that implement a variety of commonly used representations of OA sources and chemistry, as well as of the AeroCom-II ensemble. The current model ensemble captures the average vertical and spatial distribution of measured OA concentrations, and the spread of the individual models remains within a factor of 5. These results are significantly improved over the AeroCom-II model ensemble, which shows large overestimations over these regions. However, some of the improved agreement with observations occurs for the wrong reasons, as models have the tendency to greatly overestimate the primary OA fraction and underestimate the secondary fraction. Measured OA in the remote free troposphere is highly oxygenated, with organic aerosol to organic carbon (OA ∕ OC) ratios of ∼2.2–2.8, and is 30 %–60 % more oxygenated than in current models, which can lead to significant errors in OA concentrations. The model–measurement comparisons presented here support the concept of a more dynamic OA system as proposed by Hodzic et al. (2016), with enhanced removal of primary OA and a stronger production of secondary OA in global models needed to provide better agreement with observations.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-20-4607-2020
    DOI: 10.5194/acp-20-4607-2020-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
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  • 10
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    A Multimodel Investigation of Asian Summer Monsoon UTLS Transport Over the Western Pacific
    American Geophysical Union (AGU) ; 2022
    In:  Journal of Geophysical Research: Atmospheres Vol. 127, No. 24 ( 2022-12-27)
    Details
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 127, No. 24 ( 2022-12-27)
    Abstract: This model study is conducted in preparation for an airborne field campaign investigating the Asian monsoon transport Result shows that eastward eddy shedding of the anticyclone significantly alters upper tropospheric composition over the Western Pacific CO seasonal distribution provides a chemical perspective of the monsoon system and sheds new light on monsoon dynamics and circulation
    Type of Medium: Online Resource
    ISSN: 2169-897X , 2169-8996
    URL: Article
    DOI: 10.1029/2022JD037511
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2022
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