Organic aerosol (OA) in the atmosphere consists of a multitude of organic species which are either directly emitted or the products of a variety of chemical reactions. This complexity challenges our ...ability to explicitly characterize the chemical composition of these particles. We find that the bulk composition of OA from a variety of environments (laboratory and field) occupies a narrow range in the space of a Van Krevelen diagram (H:C versus O:C), characterized by a slope of ∼−1. The data show that atmospheric aging, involving processes such as volatilization, oxidation, mixing of air masses or condensation of further products, is consistent with movement along this line, producing a more oxidized aerosol. This finding has implications for our understanding of the evolution of atmospheric OA and representation of these processes in models.
We use in situ observations from the Interagency Monitoring of PROtected Visual Environments (IMPROVE) network, the Midwest Ammonia Monitoring Project, 11 surface site campaigns as well as Infrared ...Atmospheric Sounding Interferometer (IASI) satellite measurements with the GEOS-Chem model to investigate inorganic aerosol loading and atmospheric ammonia concentrations over the United States. IASI observations suggest that current ammonia emissions are underestimated in California and in the springtime in the Midwest. In California this underestimate likely drives the underestimate in nitrate formation in the GEOS-Chem model. However in the remaining continental United States we find that the nitrate simulation is biased high (normalized mean bias > = 1.0) year-round, except in Spring (due to the underestimate in ammonia in this season). None of the uncertainties in precursor emissions, the uptake efficiency of N2O5 on aerosols, OH concentrations, the reaction rate for the formation of nitric acid, or the dry deposition velocity of nitric acid are able to explain this bias. We find that reducing nitric acid concentrations to 75% of their simulated values corrects the bias in nitrate (as well as ammonium) in the US. However the mechanism for this potential reduction is unclear and may be a combination of errors in chemistry, deposition and sub-grid near-surface gradients. This "updated" simulation reproduces PM and ammonia loading and captures the strong seasonal and spatial gradients in gas-particle partitioning across the United States. We estimate that nitrogen makes up 15−35% of inorganic fine PM mass over the US, and that this fraction is likely to increase in the coming decade, both with decreases in sulfur emissions and increases in ammonia emissions.
Primary biological aerosol particles (PBAPs) may play an important role in aerosol–climate interactions, in particular by affecting ice formation in mixed phase clouds. However, the role of PBAPs is ...poorly understood because the sources and distribution of PBAPs in the atmosphere are not well quantified. Here we include emissions of fungal spores and bacteria in a global aerosol microphysics model and explore their contribution to concentrations of supermicron particle number, cloud condensation nuclei (CCN) and immersion freezing rates. Simulated surface annual mean concentrations of fungal spores are ~ 2.5 × 104 m−3 over continental midlatitudes and 1 × 105 m−3 over tropical forests. Simulated surface concentrations of bacteria are 2.5 × 104 m−3 over most continental regions and 5 × 104 m−3 over grasslands of central Asia and North America. These simulated surface number concentrations of fungal spores and bacteria are broadly in agreement with the limited available observations. We find that fungal spores and bacteria contribute 8 and 5% respectively to simulated continental surface mean supermicron number concentrations, but have very limited impact on CCN concentrations, altering regional concentrations by less than 1%. In agreement with previous global modelling studies, we find that fungal spores and bacteria contribute very little (3 × 10−3%, even when we assume upper limits for ice nucleation activity) to global average immersion freezing ice nucleation rates, which are dominated by soot and dust. However, at lower altitudes (400 to 600 hPa), where warmer temperatures mean that soot and dust may not nucleate ice, we find that PBAP controls the immersion freezing ice nucleation rate. This demonstrates that PBAPs can be of regional importance for IN formation, in agreement with case study observations.
Air pollution variability is strongly dependent on meteorology. However, quantifying the impacts of changes in regional climatology on pollution extremes can be difficult due to the many non-linear ...and competing meteorological influences on the production, transport, and removal of pollutant species. Furthermore, observed pollutant levels at many sites show sensitivities at the extremes that differ from those of the overall mean, indicating relationships that would be poorly characterized by simple linear regressions. To address this challenge, we apply quantile regression to observed daily ozone (O3) and fine particulate matter (PM2.5) levels and reanalysis meteorological fields in the USA over the past decade to specifically identify the meteorological sensitivities of higher pollutant levels. From an initial set of over 1700 possible meteorological indicators (including 28 meteorological variables with 63 different temporal options), we generate reduced sets of O3 and PM2.5 indicators for both summer and winter months, analyzing pollutant sensitivities to each for response quantiles ranging from 2 to 98 %. Primary covariates connected to high-quantile O3 levels include temperature and relative humidity in the summer, while winter O3 levels are most commonly associated with incoming radiation flux. Covariates associated with summer PM2.5 include temperature, wind speed, and tropospheric stability at many locations, while stability, humidity, and planetary boundary layer height are the key covariates most frequently associated with winter PM2.5. We find key differences in covariate sensitivities across regions and quantiles. For example, we find nationally averaged sensitivities of 95th percentile summer O3 to changes in maximum daily temperature of approximately 0.9 ppb degree C-1, while the sensitivity of 50th percentile summer O3 (the annual median) is only 0.6 ppb degree C-1. This gap points to differing sensitivities within various percentiles of the pollutant distribution, highlighting the need for statistical tools capable of identifying meteorological impacts across the entire response spectrum.
We use a suite of satellite observations (Moderate Resolution Imaging Spectroradiometer (MODIS), Multiangle Imaging Spectroradiometer (MISR), Cloud‐Aerosol Lidar With Orthogonal Polarization ...(CALIOP)) to investigate the processes of long‐range transport of dust represented in the global GEOS‐Chem model in 2006–2008. A multiyear mean of African dust transport is developed and used to test the representation of the variability in the model. We find that both MODIS and MISR correlate well with the majority of Aerosol Robotic Network observations in the region (r> 0.8). However, MODIS aerosol optical depth (AOD) appears to be biased low (>0.05) relative to MISR in Saharan regions during summer. We find that GEOS‐Chem captures much of the variability in AOD when compared with MISR and MODIS (r> 0.6) and represents the vertical structure in aerosol extinction over outflow regions well when compared to CALIOP. Including a realistic representation of the submicron‐size distribution of dust reduces simulated AOD by ∼25% over North Africa and improves agreement with observations. The lifetime of the simulated dust is typically a few days (25%–50%) shorter than inferred from MODIS observations, suggesting overvigorous wet removal, confirmed by comparison with rain rate observations from the Tropical Rainfall Measuring Mission satellite. The simulation captures the seasonality of deposition in Florida and the observed magnitude and variability of dust concentrations at Barbados from 2006 to 2008 (r = 0.74), indicating a good simulation of the impacts of North African dust on air quality in North America. We estimate that 218 ± 48 Tg of dust is annually deposited into the Atlantic and calculate a lower estimate for the dust deposited in the Caribbean and Amazon to be 26 ± 5 Tg yr−1 and 17 ± 5 Tg yr−1, respectively. This suggests that the dust deposition in the Amazon derived from satellites may be an upper limit.
Key Points
A better size representation of dust aerosol for dust optics
Climatology of African mineral dust emissions from daily to annual time scales
Estimates of dust deposition to the Americas and related uncertainties
Fine particulate matter (PM2.5) from U.S. anthropogenic sources is decreasing. However, previous studies have predicted that PM2.5 emissions from wildfires will increase in the midcentury to next ...century, potentially offsetting improvements gained by continued reductions in anthropogenic emissions. Therefore, some regions could experience worse air quality, degraded visibility, and increases in population‐level exposure. We use global climate model simulations to estimate the impacts of changing fire emissions on air quality, visibility, and premature deaths in the middle and late 21st century. We find that PM2.5 concentrations will decrease overall in the contiguous United States (CONUS) due to decreasing anthropogenic emissions (total PM2.5 decreases by 3% in Representative Concentration Pathway RCP 8.5 and 34% in RCP4.5 by 2100), but increasing fire‐related PM2.5 (fire‐related PM2.5 increases by 55% in RCP4.5 and 190% in RCP8.5 by 2100) offsets these benefits and causes increases in total PM2.5 in some regions. We predict that the average visibility will improve across the CONUS, but fire‐related PM2.5 will reduce visibility on the worst days in western and southeastern U.S. regions. We estimate that the number of deaths attributable to total PM2.5 will decrease in both the RCP4.5 and RCP8.5 scenarios (from 6% to 4–5%), but the absolute number of premature deaths attributable to fire‐related PM2.5 will double compared to early 21st century. We provide the first estimates of future smoke health and visibility impacts using a prognostic land‐fire model. Our results suggest the importance of using realistic fire emissions in future air quality projections.
Key Points
We provide the first estimates of future smoke health and visibility impacts in the contiguous United States using a prognostic land‐fire model
Average visibility will improve across the contiguous United States, but fire PM will reduce visibility on the worst days in western and southeastern U.S. regions
The number of deaths attributable to total PM2.5 will decrease, but the number attributable to fire‐related PM2.5 will double by late 21st century
The direct radiative effect (DRE) of aerosols, which is the instantaneous radiative impact of all atmospheric particles on the Earth's energy balance, is sometimes confused with the direct radiative ...forcing (DRF), which is the change in DRE from pre-industrial to present-day (not including climate feedbacks). In this study we couple a global chemical transport model (GEOS-Chem) with a radiative transfer model (RRTMG) to contrast these concepts. We estimate a global mean all-sky aerosol DRF of −0.36 Wm−2 and a DRE of −1.83 Wm−2 for 2010. Therefore, natural sources of aerosol (here including fire) affect the global energy balance over four times more than do present-day anthropogenic aerosols. If global anthropogenic emissions of aerosols and their precursors continue to decline as projected in recent scenarios due to effective pollution emission controls, the DRF will shrink (−0.22 Wm−2 for 2100). Secondary metrics, like DRE, that quantify temporal changes in both natural and anthropogenic aerosol burdens are therefore needed to quantify the total effect of aerosols on climate.
We use a global coupled chemistry-climate-land model (CESM) to assess the integrated effect of climate, emissions and land use changes on annual surface O3 and PM2.5 in the United States with a focus ...on national parks (NPs) and wilderness areas, using the RCP4.5 and RCP8.5 projections. We show that, when stringent domestic emission controls are applied, air quality is predicted to improve across the US, except surface O3 over the western and central US under RCP8.5 conditions, where rising background ozone counteracts domestic emission reductions. Under the RCP4.5 scenario, surface O3 is substantially reduced (about 5 ppb), with daily maximum 8 h averages below the primary US Environmental Protection Agency (EPA) National Ambient Air Quality Standards (NAAQS) of 75 ppb (and even 65 ppb) in all the NPs. PM2.5 is significantly reduced in both scenarios (4 mu g m-3; similar to 50%), with levels below the annual US EPA NAAQS of 12 mu g m-3 across all the NPs; visibility is also improved (10-15 dv; >75 km in visibility range), although some western US parks with Class I status (40-74 % of total sites in the US) are still above the 2050 planned target level to reach the goal of natural visibility conditions by 2064. We estimate that climate-driven increases in fire activity may dominate summertime PM2.5 over the western US, potentially offsetting the large PM2.5 reductions from domestic emission controls, and keeping visibility at present-day levels in many parks. Our study indicates that anthropogenic emission patterns will be important for air quality in 2050. However, climate and land use changes alone may lead to a substantial increase in surface O3 (2-3 ppb) with important consequences for O3 air quality and ecosystem degradation at the US NPs. Our study illustrates the need to consider the effects of changes in climate, vegetation, and fires in future air quality management and planning and emission policy making.
The Galactic Faraday rotation sky 2020 Hutschenreuter, S.; Anderson, C. S.; Betti, S. ...
Astronomy and astrophysics (Berlin),
01/2022, Letnik:
657
Journal Article
Recenzirano
Odprti dostop
Aims.
This work provides an update to existing reconstructions of the Galactic Faraday rotation sky by processing almost all Faraday rotation data sets available at the end of the year 2020. ...Observations of extra-Galactic sources in recent years have further illuminated the previously underconstrained southern celestial sky, as well as parts of the inner disc of the Milky Way, along with other regions. This has culminated in an all-sky data set of 55 190 data points, thereby comprising a significant expansion on the 41 330 used in previous works. At the same time, this novelty makes an updated separation of the Galactic component a promising enterprise. The increased source density allows us to present our results in a resolution of about 1.3 × 10
−2
deg
2
(46.8 arcmin
2
), which is a twofold increase compared to previous works.
Methods.
As for previous Faraday rotation sky reconstructions, this work is based on information field theory, namely, a Bayesian inference scheme for field-like quantities that handles noisy and incomplete data.
Results.
In contrast to previous reconstructions, we find a significantly thinner and pronounced Galactic disc with small-scale structures exceeding values of several thousand rad m
−2
. The improvements can mainly be attributed to the new catalog of Faraday data, but are also supported by advances in correlation structure modeling within numerical information field theory. We also provide a detailed discussion on the statistical properties of the Faraday rotation sky and we investigate correlations with other data sets.
We discuss and evaluate the representation of atmospheric chemistry in the global Community Atmosphere Model (CAM) version 4, the atmospheric component of the Community Earth System Model (CESM). We ...present a variety of configurations for the representation of tropospheric and stratospheric chemistry, wet removal, and online and offline meteorology. Results from simulations illustrating these configurations are compared with surface, aircraft and satellite observations. Major biases include a negative bias in the high-latitude CO distribution, a positive bias in upper-tropospheric/lower-stratospheric ozone, and a positive bias in summertime surface ozone (over the United States and Europe). The tropospheric net chemical ozone production varies significantly between configurations, partly related to variations in stratosphere-troposphere exchange. Aerosol optical depth tends to be underestimated over most regions, while comparison with aerosol surface measurements over the United States indicate reasonable results for sulfate , especially in the online simulation. Other aerosol species exhibit significant biases. Overall, the model-data comparison indicates that the offline simulation driven by GEOS5 meteorological analyses provides the best simulation, possibly due in part to the increased vertical resolution (52 levels instead of 26 for online dynamics). The CAM-chem code as described in this paper, along with all the necessary datasets needed to perform the simulations described here, are available for download at www.cesm.ucar.edu.
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