Title: AERO-MAP: a data compilation and modeling approach to understand spatial variability in fine- and coarse-mode aerosol composition
Abstract. Aerosol particles are an important part of the Earth climate system, and their concentrations are spatially and temporally heterogeneous, as well as being variable in size and composition. Particles can interact with incoming solar radiation and outgoing longwave radiation, change cloud properties, affect photochemistry, impact surface air quality, change the albedo of snow and ice, and modulate carbon dioxide uptake by the land and ocean. High particulate matter concentrations at the surface represent an important public health hazard. There are substantial data sets describing aerosol particles in the literature or in public health databases, but they have not been compiled for easy use by the climate and air quality modeling community. Here, we present a new compilation of PM2.5 and PM10 surface observations, including measurements of aerosol composition, focusing on the spatial variability across different observational stations. Climate modelers are constantly looking for multiple independent lines of evidence to verify their models, and in situ surface concentration measurements, taken at the level of human settlement, present a valuable source of information about aerosols and their human impacts complementarily to the column averages or integrals often retrieved from satellites. We demonstrate a method for comparing the data sets to outputs from global climate models that are the basis for projections of future climate and large-scale aerosol transport patterns that influence local air quality. Annual trends and seasonal cycles are discussed briefly and are included in the compilation. Overall, most of the planet or even the land fraction does not have sufficient observations of surface concentrations – and, especially, particle composition – to characterize and understand the current distribution of particles. Climate models without ammonium nitrate aerosols omit ∼ 10 % of the globally averaged surface concentration of aerosol particles in both PM2.5 and PM10 size fractions, with up to 50 % of the surface concentrations not being included in some regions. In these regions, climate model aerosol forcing projections are likely to be incorrect as they do not include important trends in short-lived climate forcers.  more » « less
Award ID(s):
2215875 2020673
PAR ID:
10628522
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; more » ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; « less
Publisher / Repository:
Atmospheric Chemistry and Physics
Date Published:
Journal Name:
Atmospheric Chemistry and Physics
Volume:
25
Issue:
9
ISSN:
1680-7324
Page Range / eLocation ID:
4665 to 4702
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Rapid warming is likely increasing primary production and wildfire occurrence in the Arctic. Projected changes in the abundance and composition of carbonaceous aerosols during the summer are likely to impact atmospheric chemistry and climate, but our understanding of these processes is limited by sparse observations. Here, we characterize carbonaceous aerosol at two field sites, Toolik Field Station in the Interior and the Atmospheric Radiation Measurement facility at Utqiaġvik on the Arctic coast of Alaska, USA, through the summers of 2022 and 2023. We estimated particulate matter ≤2.5 micrometers (PM2.5) and particulate matter ≤10 micrometers (PM10) using laser light scattering (PurpleAir sensors) and examined total carbon (TC) and its organic carbon (OC) and elemental carbon (EC) fractions in total suspended particles (TSP). We also investigated the dominant sources of carbonaceous aerosol using air mass backward-trajectories from the National Oceanic and Atmospheric Administration (NOAA) Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model and radiocarbon source apportionment of TC. We found TC concentrations were about twice as high in the Interior than on the coast and that modern sources were the dominant sources of carbonaceous aerosol at both Toolik (95–99%) and Utqiaġvik (86–89%), with minor contributions from fossil sources. Periods of significantly elevated PM, TC, OC, and EC concentrations coincided with major boreal forest fire activity in North America that brought smoke to the region. The radiocarbon signature of EC measured at Toolik during these wildfire smoke events indicated that over 90% of the EC originated from modern sources. Our measurements demonstrate changing aerosol concentrations in the Arctic during the summer, and emphasize the need for continuous atmospheric monitoring to evaluate and advance our understanding of this rapidly changing atmospheric environment. (Manuscript in prep) 
    more » « less
  2. Rapid warming is likely increasing primary production and wildfire occurrence in the Arctic. Projected changes in the abundance and composition of carbonaceous aerosols during the summer are likely to impact atmospheric chemistry and climate, but our understanding of these processes is limited by sparse observations. Here, we characterize carbonaceous aerosol at two field sites, Toolik Field Station in the Interior and the Atmospheric Radiation Measurement facility at Utqiaġvik on the Arctic coast of Alaska, USA, through the summers of 2022 and 2023. We estimated particulate matter ≤2.5 micrometers (PM2.5) and particulate matter ≤10 micrometers (PM10) using laser light scattering (PurpleAir sensors) and examined total carbon (TC) and its organic carbon (OC) and elemental carbon (EC) fractions in total suspended particles (TSP). We also investigated the dominant sources of carbonaceous aerosol using air mass backward-trajectories from the National Oceanic and Atmospheric Administration (NOAA) Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model and radiocarbon source apportionment of TC. We found TC concentrations were about twice as high in the Interior than on the coast and that modern sources were the dominant sources of carbonaceous aerosol at both Toolik (95–99%) and Utqiaġvik (86–89%), with minor contributions from fossil sources. Periods of significantly elevated PM, TC, OC, and EC concentrations coincided with major boreal forest fire activity in North America that brought smoke to the region. The radiocarbon signature of EC measured at Toolik during these wildfire smoke events indicated that over 90% of the EC originated from modern sources. Our measurements demonstrate changing aerosol concentrations in the Arctic during the summer, and emphasize the need for continuous atmospheric monitoring to evaluate and advance our understanding of this rapidly changing atmospheric environment. (Manuscript in prep) 
    more » « less
  3. Understanding new particle formation (NPF) and the fate of nanoparticles is crucial because of their close links to air quality, cloud formation, and climate. These effects vary spatially and temporally owing to diverse aerosol sources and their relatively short atmospheric lifetime. Here, we present a comprehensive analysis of long-term trends in NPF-associated nucleation-mode particles and cloud condensation nuclei (CCN) concentrations across diverse observation environments using quality-controlled particle number size distribution (PNSD) and CCN data from 37 sites, primarily from Global Atmosphere Watch (GAW) stations. We identify declining decadal trends in both NPF occurrences and nucleated particle concentrations across most site types, with the strongest declines in urban areas. We observe simultaneous reductions in both CCN concentrations and nucleation-mode particles, suggesting that newly formed particles are a potential source of CCN. This, in turn, suggests that cloud microphysical properties and radiative effects can be indirectly influenced through aerosol−cloud interactions that modify cloud droplet formation. These findings indicate that decreasing anthropogenic emissions could influence the climate forcing potential of aerosol−cloud interactions, with important implications for future climate projections. 
    more » « less
  4. Abstract Incoming surface shortwave radiation () has exhibited regionally‐variable multidecadal trends and variability over land that have variously been linked to aerosols and clouds. However, limitations in the spatiotemporal coverage of the observations, combined with apparent disagreements between climate models and observations, have precluded global analyses. Here, we first demonstrate that both the variability and trends in ERA5 agree favorably with high‐quality estimates from satellite and in situ sources, and then show evidence of substantial continental brightening from 1980 to 2024, including in places like the central United States, Brazil, and central Asia that do not show large trends in aerosol concentrations over the same period. The brightening in these regions is co‐located with reductions in total cloud cover, and trends in both are at the edge or entirely outside an ensemble of 237 CMIP6‐era climate model simulations, whose spatial pattern of trends more directly reflect the pattern of aerosol concentrations. 
    more » « less
  5. Sea salt aerosols are known to serve as effective cloud condensation nuclei and are prominent contributors of light scattering in the atmosphere. More light scattering reduces solar radiations to the Earth and lowers the global temperature. Researchers observed that ambient sea salt aerosols may contain ammonium sulfate (AS) and sodium chloride (NaCl). Recent studies showed that alkylamines, derivatives of ammonia, can react with ammonium salts in the aerosol, displacing ammonium and altering the particle’s properties. Our study investigated the effects of atmospheric alkylamines on the properties of sea salt aerosols using a chemical system of methylamine (MA), AS, and NaCl. We determined the relative humidity when these aerosols start to absorb water vapor from the air (deliquescent relative humidity, DRH), and concentrations of ammonia and MA in aqueous/gas phases using the Extended Aerosols and Inorganics Model. Our findings indicate a notable negative relationship between MA concentration and the DRH for both AS and NaCl. We determined that five parts per billion or higher of MA effectively lowered the DRH of sea salt aerosol particles. The concentrations of ammonia and MA in aqueous and gas phases had a complex dependence on MA concentration and aerosol chemical composition. Aerosol deliquescence often leads to cloud/fog processing which may cool the Earth by reflecting sunlight away from the surface. Therefore, our results implicate a potential role for alkylamines in climate change, suggesting the importance of monitoring alkylamine concentrations in the atmosphere. Future studies are needed to better predict the deliquescent behaviors of aerosols, namely particles containing AS and NaCl, such as those found near coasts. 
    more » « less