Even though desert dust is the most abundant aerosol by mass in Earth’s atmosphere, atmospheric models 25 struggle to accurately represent its spatial and temporal distribution. These model errors ...are partially caused byfundamental difficulties in simulating dust emission in coarse-resolution models and in accurately representing dust microphysical properties. Here we mitigate these problems by developing a new methodology that yields an improved representation of the global dust cycle. We present an analytical framework that uses inverse modeling to integrate an ensemble of global model simulations with observational constraints on the dust size distribution, 30 extinction efficiency, and regional dust aerosol optical depth. We then compare the inverse model results against independent measurements of dust surface concentration and deposition flux and find that errors are reduced by approximately a factor of two relative to current model simulations of the Northern Hemisphere dust cycle. The inverse model results show smaller improvements in the less dusty Southern Hemisphere, most likely because both the model simulations and the observational constraints used in the inverse model are less accurate. On a global 35 basis, we find that the emission flux of dust with geometric diameter up to 20 μm (PM20) is approximately 5,000 Tg/year, which is greater than most models account for. This larger PM20 dust flux is needed to match observational constraints showing a large atmospheric loading of coarse dust. We obtain gridded data sets of dust emission, vertically integrated loading, dust aerosol optical depth, (surface) concentration, and wet and dry deposition fluxes that are resolved by season and particle size. As our results indicate that this data set is more accurate than current 40 model simulations and the MERRA-2 dust reanalysis product, it can be used to improve quantifications of dust impacts on the Earth system.
Interactions of meteorology with wildfires in British Columbia, Canada during August 2017 led to three
major pyrocumulonimbus (pyroCb) events that resulted in the injection of large amounts of smoke ...aerosols and other combustion products at the local upper troposphere and lower stratosphere (UTLS). These plumes of UTLS smoke
with elevated values of aerosol extinction and backscatter compared to the background state were readily tracked by
multiple satellite-based instruments as they spread across the Northern Hemisphere (NH). The plumes were observed
in the lower stratosphere for about 8-10 months following the fire injections, with a stratospheric aerosol e-folding
time of about 5 months. To investigate the radiative impacts of these events on the Earth system, we performed a number of simulations with the Goddard Earth Observing System (GEOS) atmospheric general circulation model
(AGCM). Observations from multiple remote-sensing instruments were used to calibrate the injection parameters
(location, amount, composition and heights) and optical properties of the smoke aerosols in the model. The resulting
simulations of three-dimensional smoke transport were evaluated for a year from the day of injections using daily
observations from OMPS-LP (Ozone Mapping Profiler Suite Limb Profiler). The model simulated rate of ascent, hemispheric spread and residence time (or e-folding time) of the smoke aerosols in the stratosphere are in close
agreement with OMPS-LP observations. We found that both aerosol self-lofting and the large-scale atmospheric motion play important roles in lifting the smoke plumes from near the tropopause altitudes (~12 km) to about 22-23
km into the atmosphere. Further, our estimations of the radiative impacts of the pyroCb-emitted smoke aerosols showed that the smoke caused an additional warming of the atmosphere by about 0.6-1 W/m2 (zonal mean) that persisted for about 2-3 months after the injections in regions north of 40oN. The surface experienced a comparable
magnitude of cooling. The atmospheric warming is mainly located in the stratosphere, coincident with the location of the smoke plumes, leading to an increase in zonal mean shortwave (SW) heating rates of 0.02-0.04 K/day during
September 2017.
In order to improve aerosol representation in the NASA Goddard Earth Observing System (GEOS) model, we evaluated simulations of the aerosol properties and transport over the southern African biomass ...burning source and outflow region using observations made during the first deployment of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) field campaign in September 2016. An example case study of September 24 was analyzed in detail, during which aircraft-based in-situ and remote sensing observations showed the presence of a multi-layered smoke plume structure with significant vertical variation in single scattering albedo (SSA). Our baseline GEOS simulations were not able to represent the observed SSA variation, nor the observed organic aerosol-to-black carbon ratio (OA : BC). Analyzing the simulated smoke age suggests that the higher altitude, less absorbing smoke plume was younger (~4 days), while the lower altitude and more absorbing smoke plume was older (~7 days). We hypothesize a chemical or microphysical loss process exists to explain the change in aerosol absorption as the smoke plume ages, and we apply a simple 6-day e-folding loss rate to the model hydrophilic biomass burning OA to mimic this process. Adding this loss process required some adjustment to the model assumed scaling factors of aerosol emissions to conserve the regional aerosol loading and further improve the simulated OA : BC ratio. Accordingly, we have increased our biomass burning emissions of OA by 60 % and biomass burning BC by 15 %. We also utilized the ORACLES airborne observations to better constrain the simulation of aerosol optical properties, adjusting the assumed particle size, hygroscopic growth, and absorption. Our final GEOS model simulation with additional OA loss and updated optics showed a better performance in simulating AOD and SSA compared to independent ground and space-based retrievals for the entire month of September 2016, including the OMI Aerosol Index. In terms of radiative implications of our model adjustments, the final GEOS simulation suggested a decreased atmospheric warming of about 10 % (~2 W m-2) over the south-east Atlantic region and above the stratocumulus cloud decks compared to the model baseline simulations. These results improve the representation of the smoke age, transport, and optical properties in Earth system models.
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.
International Cooperative for Aerosol Predictions (ICAP) model 550 nm total AOD RMSE of the 72 h forecast versus corresponding mean AODs for AERONET sites listed in Table 2. Large black dots are ICAP multi‐model ensemble consensus means. Individual models are in small coloured dots. Validation of fine‐ and coarse‐modal AODs and dust AOD is also available in Figure 2.
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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.
Atmospheric sea salt plays important roles in marine cloud formation and
atmospheric chemistry. We performed an integrated analysis of NASA GEOS
model simulations run with the GOCART aerosol module, ...in situ measurements from the PALMS and SAGA instruments obtained during the NASA ATom campaign, and aerosol optical depth (AOD) measurements from the AERONET Marine Aerosol Network (MAN) and from MODIS satellite observations to better constrain sea salt in the marine atmosphere. ATom measurements and GEOS model simulations both show that sea salt concentrations over the Pacific and Atlantic oceans have a strong vertical gradient, varying up to 4 orders of magnitude from the marine boundary layer to free troposphere. The modeled residence times suggest that the lifetime of sea salt particles with a dry diameter of less than 3 µm is largely controlled by wet removal, followed by turbulent process. During both boreal summer and winter, the GEOS-simulated sea salt mass mixing ratios agree with SAGA measurements in the marine boundary layer (MBL) and with PALMS measurements above the MBL. However, comparison of AOD from GEOS with AERONET/MAN and MODIS aerosol retrievals indicated that the model underestimated AOD over the oceans where sea salt dominates. The apparent discrepancy of slightly overpredicted concentration and large underpredicted AOD could not be explained by biases in the model RH affecting the particle hygroscopic growth, as modeled RH was found to be
comparable to or larger than the in situ measurements. This conundrum could at least partially be explained by the difference in sea salt size distribution; the GEOS simulation has much less sea salt percentage-wise in the smaller particle size range and thus less efficient light extinction than what was observed by PALMS.
The Pacific Northwest pyrocumulonimbus Event (PNE) took place in British Columbia during the evening and night-time hours between the 12th and 13th of August 2017. Several pyroconvective clouds ...erupted in this occasion, and released in the upper troposphere/lower stratosphere unprecedented amounts of carbonaceous aerosols (300 ktn). Only a few years later, an even larger pyroCb injection took place over Australia. This event, named the Australian New Year (ANY) event, injected up to 1100 ktn of aerosol between December 29th 2019 and January 4th 2020. Such large injections of carbonaceous aerosol modify the stratospheric radiative budgets, locally perturbing stratospheric temperatures and winds. In this study, we use the Goddard Earth Observing System Chemistry Climate Model (GEOS CCM) to study the pertubations on the stratospheric meteorology induced by an aerosol injection of the magnitude of the PNE. Our simulations include the radiative interactions of aerosols, so that their impact on temperatures and winds are explicitly simulated. We show how the presence of the carbonaceous aerosols from the pyroCb causes the formation and maintenance of a synoptic scale stratospheric anticyclone. We follow this disturbance considering the potential vorticity anomaly and the brown carbon aerosol loading and we describe its dynamical and thermodynamical structure and its evolution in time. The analysis presented here shows that the simulated anticyclone undergoes daily expansion-compression cycles governed by the radiative heating, which are directly related to the vertical motion of the plume, and that the aerosol radiative heating is essential in maintaining the anticyclone itself.
The Chilean volcano Cerro Hudson erupted between August 8th and 15th, 1991, injecting between 1.7 and 2.9 Tg of SO2 into the upper troposphere and lower stratosphere. We simulate this injection using ...the Goddard Earth Observing System Earth system model with detailed sulfur chemistry and sectional aerosol microphysics, focusing on the resulting aerosols and their contribution to the 1991 Antarctic Austral Springtime ozone hole. The simulations show a column ozone deficit (12 DU) in the Southern Hemisphere vortex collar region. The majority of this effect is between 10 and 20 km and due to heterogeneous chemistry. The model shows a 26% decrease in ozone from background levels at these altitudes, compared with in‐situ observations of a 50% decrease. Above 20 km, the dynamical response to the eruption also causes lower ozone values, a novel modeling result. This experiment highlights potential interactions between proposed solar radiation management geoengineering aerosols and volcanic eruptions.
Plain Language Summary
We simulated the August 1991 eruption of Chilean volcano Cerro Hudson. Cerro Hudson erupted 2 months after the June 15th eruption of Pinatubo which was one of the largest observed eruptions. The combination of these two eruptions impacted the atmosphere by injecting volcanic aerosol which are well represented by our model. In the case of Cerro Hudson, the simulations show that the volcanic plume may have impacted the 1991 Antarctic ozone hole, both by directly impacting the chemistry of ozone depletion and by altering the dynamics of the atmosphere, slowing down the normal breakdown of the ozone hole caused by changes in weather. The interaction between Cerro Hudson and Pinatubo shown here also reveal a need for more research in how potential goengineering scenarios would interact with volcanic eruptions.
Key Points
The August 1991 eruption of Cerro Hudson is simulated using a model with detailed aerosol microphysics and stratospheric chemistry
The model shows skill in simulating the satellite and in‐situ observations of the volcanic plume
These simulations present a prima facie case that this eruption contributed to the anomalously high 1991 Austral Springtime ozone loss
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North African dust reaches the southeastern United States every summer. Size-resolved dust mass measurements taken in Miami, Florida, indicate that more than one-half of the surface dust mass ...concentrations reside in particles with geometric diameters less than 2.1 µm, while vertical profiles of micropulse lidar depolarization ratios show dust reaching above 4 km during pronounced events. These observations are compared to the representation of dust in the Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) aerosol reanalysis and closely related Goddard Earth Observing System model version 5 (GEOS-5) Forward Processing (FP) aerosol product, both of which assimilate satellite-derived aerosol optical depths using a similar protocol and inputs. These capture the day-to-day variability in aerosol optical depth well, in a comparison to an independent sun-photometer-derived aerosol optical depth dataset. Most of the modeled dust mass resides in diameters between 2 and 6 µm, in contrast to the measurements. Model-specified mass extinction efficiencies equate light extinction with approximately 3 times as much aerosol mass, in this size range, compared to the measured dust sizes. GEOS-5 FP surface-layer sea salt mass concentrations greatly exceed observed values, despite realistic winds and relative humidities. In combination, these observations help explain why, despite realistic total aerosol optical depths, (1) free-tropospheric model volume extinction coefficients are lower than those retrieved from the micro-pulse lidar, suggesting too-low model dust loadings in the free troposphere, and (2) model dust mass concentrations near the surface can be higher than those measured. The modeled vertical distribution of dust, when captured, is reasonable. Large, aspherical particles exceeding the modeled dust sizes are also occasionally present, but dust particles with diameters exceeding 10 µm contribute little to the measured total dust mass concentrations after such long-range transport. Remaining uncertainties warrant a further integrated assessment to confirm this study's interpretations.
The radiative effects of Saharan dust aerosols are investigated in the NASA GEOS‐5 atmospheric general circulation model. A sectional aerosol microphysics model (CARMA) is run online in GEOS‐5. CARMA ...treats the dust aerosol lifecycle, and its tracers are radiatively coupled to GEOS‐5. A series of AMIP‐style simulations are performed, in which input dust optical properties (particle shape and refractive index) are varied. Simulated dust distributions for summertime Saharan dust compare well to observations, with best results found when the most absorbing dust optical properties are assumed. Dust absorption leads to a strengthening of the summertime Hadley cell circulation, increased dust lofting to higher altitudes, and a strengthening of the African easterly jet, resulting in increased dust atmospheric lifetime and farther northward and westward transport. We find a positive feedback of dust radiative forcing on emissions, in contrast with previous studies, which we attribute to our having a relatively strong longwave forcing caused by our simulating larger effective particle sizes. This longwave forcing reduces the magnitude of midday net surface cooling relative to other studies, and leads to a nighttime warming that results in higher nighttime wind speeds and dust emissions. The radiative effects of dust particle shape have only minor impact on transport and emissions, with small (~5%) impact on top of atmosphere shortwave forcing, in line with previous studies, but relatively more pronounced effects on shortwave atmospheric heating and surface forcing (~20% increase in atmospheric forcing for spheroids). Shape effects on longwave heating terms are of order ~10%.
Key Points
Dust absorption has a positive feedback on dust emissions
Stronger absorption leads to longer range transport of dust aerosols
Dust forcing impacts are more tied to refractive index than particle shape
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