An investigation of volcanic gases and dust (aerosols) in the stratosphere
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Approximately 240 Tg of mineral dust aerosol are transported annually from Saharan Africa to the Atlantic Ocean. Dust affects the Earth radiation budget, and plays direct (through scattering and absorption of radiation) and indirect (through modification of cloud properties and environment) roles in climate. Deposition of dust to the surface provides an important nutrient source to terrestrial and oceanic ecosystems. Dust is additionally a contributor to adverse air quality. Among the tools toward understanding the lifecycle and impacts of mineral dust aerosols are numerical models. Important constraints on these models come from quantitative satellite observations, like those from the space-based Moderate Resolution Imaging Spectroradiometer (MODIS). In particular, Kauhan et al. [2005] used MODIS aerosol observations to infer transport and deposition fluxes of Saharan dust over the Atlantic, Caribbean, and Amazonian basins. Those observations are used here to constrain the transport of dust and its interannual variability simulated in the NASA GEOS-5 general circulation model and data assimilation system. Significant uncertainty exists in the MODIS-derived fluxes, however, due to uncertainty in the wind fields provided by meteorological analyses in this region. That same uncertainty in the wind fields is manifest in our GEOS-5 simulations of dust distributions. Here we use MODIS observations to investigate the seasonality and location of the Saharan dust plume and explore through sensitivity analysis of our model the meteorological controls on the dust distribution, including dust direct radiative effects and sub-gridscale source and sink processes.
Emissions and long-range transport of mineral dust and combustion-related aerosol from burning fossil fuels and biomass vary from year to year, driven by the evolution of the economy and changes in meteorological conditions and environmental regulations. This study offers both satellite and model perspectives of interannual variability and possible trend of combustion aerosol and dust in major continental outflow regions over the past 15 years (2003-2017). The decade-long record of aerosol optical depth (AOD, denoted as t), separately for combustion aerosol (τ(sub c)) and dust (τ(sub d)), over global oceans is derived from the Collection 6 aerosol products of the Moderate Resolution Imaging Spectroradiometer (MODIS) onboard both Terra and Aqua. These MODIS/Aqua datasets, complemented by aerosol source-tagged simulations using the Community Atmospheric Model Version 5 (CAM5), are then analyzed to understand the interannual variability and potential trend of τ(sub c) and τ(sub d) in the major continental outflows. Both MODIS and CAM5 consistently yield a similar decreasing trend of -0.017 to - 0.020 decade(exp -1) for τ(sub c) over the North Atlantic Ocean and the Mediterranean Sea that is attributable to reduced emissions from North America and Europe, respectively. On the contrary, both MODIS and CAM5 display an increasing trend of +0.017 to +0.036 decade(exp -1) for τ(sub c) over the tropical Indian Ocean, the Bay of Bengal, and the Arabian Sea, which reflects the influence of increased anthropogenic emissions from South Asia and Middle East in the last two decades. Over the northwestern Pacific Ocean that is often affected by East Asian emissions of pollution and dust, the MODIS retrievals show a decreasing trend of - 0.021 decade(exp -1) for τ(sub c) and -0.012 decade(exp -1) for τ(sub d), which is however not reproduced by the CAM5 model. In other outflow regions strongly influenced by biomass burning smoke or dust, both MODIS retrievals and CAM5 simulations show no statistically significant trends; and the MODIS observed interannual variability is usually larger than that of the CAM5 simulation.
Massive quantities of dust aerosol, originating at source locations in the Saharan desert are frequently transported westward across the Atlantic. Saharan dust has been frequently identified at ground-based stations in South America, on Barbados, in Florida and in Texas. Recently, in July of 2000, the Puerto Rican Dust Experiment (PRiDE), consisting of researchers from the U.S. Navy, NASA, the University of Miami and the University of Puerto Rico joined together to study this important phenomenon. Numerical forecast models tracked each dust event as the dust left the African continent and transversed the Atlantic. Ground-based, ship-based, airborne and satellite sensors were used to characterize the physical and radiative properties of the dust aerosol. The dust plays an important role in terms of radiative forcing of regional climate. Satellite sensors such as NASA's EOS-MODIS aboard the Terra satellite will provide important continuing information on the dust aerosol and its climatic effects.
The formation of ice in clouds depends on the availability of ice forming nuclei (IFN). Dust aerosol particles are considered the most important source of IFN at a global scale. Recent laboratory studies have demonstrated that the mineral feldspar provides the most efficient dust IFN for immersion freezing and together with kaolinite for deposition ice nucleation, and that the phyllosilicates illite and montmorillonite (a member of the smectite group) are of secondary importance.A few studies have applied global models that simulate mineral specific dust to predict the number and geographical distribution of IFN. These studies have been based on the simple assumption that the mineral composition of soil as provided in data sets from the literature translates directly into the mineral composition of the dust aerosols. However, these tables are based on measurements of wet-sieved soil where dust aggregates are destroyed to a large degree. In consequence, the size distribution of dust is shifted to smaller sizes, and phyllosilicates like illite, kaolinite, and smectite are only found in the size range 2 m. In contrast, in measurements of the mineral composition of dust aerosols, the largest mass fraction of these phyllosilicates is found in the size range 2 m as part of dust aggregates. Conversely, the mass fraction of feldspar is smaller in this size range, varying with the geographical location. This may have a significant effect on the predicted IFN number and its geographical distribution.An improved mineral specific dust aerosol module has been recently implemented in the NASA GISS Earth System ModelE2. The dust module takes into consideration the disaggregated state of wet-sieved soil, on which the tables of soil mineral fractions are based. To simulate the atmospheric cycle of the minerals, the mass size distribution of each mineral in aggregates that are emitted from undispersed parent soil is reconstructed. In the current study, we test the null-hypothesis that simulating the presence of a large mass fraction of phyllosilicates in dust aerosols in the size range 2 m, in comparison to a simple model assumption where this is neglected, does not yield a significant effect on the magnitude and geographical distribution of the predicted IFN number. Results from sensitivity experiments are presented as well.
The atmospheric supply of mineral dust iron (Fe) plays a crucial role in the Earths biogeochemical cycle and is of specific importance as a micronutrient in the marine environment. Observations show several orders of magnitude variability in the fractional solubility of Fe in mineral dust aerosols, making it hard to assess the role of mineral dust for the global ocean biogeochemical Fe cycle. In this study we compare the operational solubility of mineral dust aerosol Fe associated with the flow-through leaching protocol to the results of the global 3-D chemical transport model GEOS-Chem. According to the protocol, aerosol Fe is defined as soluble by first deionized water leaching of mineral dust through a 0.45 m pore size membrane followed by acidification and storage of the leachate over a long period of time prior to analysis. To estimate the uncertainty in soluble Fe results introduced by the flow-through leaching protocol, we prescribe an average 50 (range of 30 to 70) fractional solubility to sub-0.45 m sized mineral dust particles that may inadvertently pass the filter and end up in the acidified (at pH1.7) leachate for a couple of month period. In the model, the fractional solubility of Fe is either explicitly calculated using a complex mineral aerosol Fe dissolution module, or prescribed to be 1 and 4. Calculations show that the fractional solubility of Fe derived through the flow-through leaching is higher compared to the model results. The largest differences (40) are predicted to occur farther away from the dust source regions, over the areas where sub-0.45 m sized mineral dust particles contribute a larger fraction of the total mineral dust mass. This study suggests that different methods used in soluble Fe measurements and inconsistences in the operational definition of filterable Fe in marine environment and soluble Fe in atmospheric aerosols are likely to contribute to the wide range of fractional solubility of aerosol Fe reported in the literature.
Numerical weather prediction systems depend on Hyperspectral Infrared Sounder (HIS) data, yet the impacts of dust-contaminated HIS radiances on weather forecasts has not been quantified. To determine the impact of dust aerosol on HIS radiance assimilation, we use a modified radiance assimilation system employing a one-dimensional variational assimilation system (1DVAR) developed under the European Organisation for the Exploitation of Meteorological Satellites (EUMETSAT) Numerical Weather Prediction–Satellite Application Facility (NWP-SAF) project, which uses the Radiative Transfer for TOVS (RTTOV). Dust aerosol impacts on analyzed temperature and moisture fields are quantified using synthetic HIS observations from rawinsonde, Micropulse Lidar Network (MPLNET), and Aerosol Robotic Network (AERONET). Specifically, a unit dust aerosol optical depth (AOD) contamination at 550 nm can introduce larger than 2.4 and 8.6 K peak biases in analyzed temperature and dewpoint, respectively, over our test domain. We hypothesize that aerosol observations, or even possibly forecasts from aerosol predication models, may be used operationally to mitigate dust induced temperature and moisture analysis biases through forward radiative transfer modeling.
Numerical weather prediction systems depend on Hyperspectral Infrared Sounder (HIS) data, yet the impacts of dust-contaminated HIS radiances on weather forecasts has not been quantified. To determine the impact of dust aerosol on HIS radiance assimilation, we use a modified radiance assimilation system employing a one-dimensional variational assimilation system (1DVAR) developed under the European Organisation for the Exploitation of Meteorological Satellites (EUMETSAT) Numerical Weather Prediction–Satellite Application Facility (NWP-SAF) project, which uses the Radiative Transfer for TOVS (RTTOV). Dust aerosol impacts on analyzed temperature and moisture fields are quantified using synthetic HIS observations from rawinsonde, Micropulse Lidar Network (MPLNET), and Aerosol Robotic Network (AERONET). Specifically, a unit dust aerosol optical depth (AOD) contamination at 550 nm can introduce larger than 2.4 and 8.6 K peak biases in analyzed temperature and dewpoint, respectively, over our test domain. We hypothesize that aerosol observations, or even possibly forecasts from aerosol predication models, may be used operationally to mitigate dust induced temperature and moisture analysis biases through forward radiative transfer modeling.
Quantification of dust aerosols in Earth System Models (ESMs) has important implications for water cycle and biogeochemistry studies. This study examines the global life cycle and direct radiative effects (DREs) of dust in the U.S. Department of Energy's Energy Exascale Earth System Model version 1 (E3SMv1), and the impact of increasing model resolution both horizontally and vertically. The default 1° E3SMv1 captures the spatial and temporal variability in the observed dust aerosol optical depth (DAOD) reasonably well, but overpredicts dust absorption in the shortwave (SW). Simulations underestimate the dust vertical and long-range transport, compared with the satellite dust extinction profiles. After updating dust refractive indices and correcting for a bias in partitioning size-segregated emissions, both SW cooling and longwave (LW) warming of dust simulated by E3SMv1 are increased and agree better with other recent studies. The estimated net dust DRE of −0.42 Wm−2 represents a stronger cooling effect than the observationally based estimate −0.2 Wm−2 (−0.48 to +0.2), due to a smaller LW warming. Constrained by a global mean DAOD, model sensitivity studies of increasing horizontal and vertical resolution show strong influences on the simulated global dust burden and lifetime primarily through the change of dust dry deposition rate; there are also remarkable differences in simulated spatial distributions of DAOD, DRE, and deposition fluxes. Thus, constraining the global DAOD is insufficient for accurate representation of dust climate effects, especially in transitioning to higher- or variable-resolution ESMs. Better observational constraints of dust vertical profiles, dry deposition, size, and LW properties are needed.
Airborne mineral dust particles can act as natural seeds for cirrus clouds in the upper troposphere. However, the atmospheric abundance of dust is unconstrained in cirrus-forming regions, hampering our ability to predict these radiatively important clouds. Here we present global-scale measurements of dust aerosol abundance in the upper troposphere and incorporate these into a detailed cirrus-formation model. We show that dust aerosol initiates cirrus clouds throughout the extra-tropics in all seasons and dominates cirrus formation in the Northern Hemisphere (75–93% of clouds seasonally). Using a global transport model with improved dust treatment, we also explore which of Earth’s deserts are the largest contributors of dust aerosol to cirrus-forming regions. We find that the meteorological environment downstream of each emission region modulates dust atmospheric lifetime and transport efficiency to the upper troposphere so that source contributions are disproportionate to emissions. Our findings establish the critical role of dust in Earth’s climate system through the formation of cirrus clouds.
In the Aerosol Robotic Network (AERONET) retrieval algorithm, smoothness constraints on the imaginary part of the refractive index provide control of retrieved spectral dependence of aerosol absorption by preventing the inversion code from fitting the noise in optical measurements and thus avoiding unrealistic oscillations of retrievals with wavelength. The history of implementation of the smoothness constraints in the AERONET retrieval algorithm is discussed. It is shown that the latest version of the smoothness constraints on the imaginary part of refractive index, termed standard and employed by Version 3 of the retrieval algorithm, should be modified to account for strong variability of light absorption by brown-carbon-containing aerosols in UV through mid-visible parts of the solar spectrum. In Version 3 strong spectral constraints were imposed at high values of the Ångström exponent (440–870 nm) since black carbon was assumed to be the primary absorber, while the constraints became increasingly relaxed as aerosol exponent deceased to allow for wavelength dependence of absorption for dust aerosols. The new version of the smoothness constraints on the imaginary part of the refractive index assigns different weights to different pairs of wavelengths, which are the same for all values of the Ångström exponent. For example, in the case of four-wavelength input, the weights assigned to short-wavelength pairs (440–675, 675–870 nm) are small so that smoothness constraints do not suppress natural spectral variability of the imaginary part of the refractive index. At longer wavelengths (870–1020 nm), however, the weight is 10 times higher to provide additional constraints on the imaginary part of refractive index retrievals of aerosols with a high Ångström exponent due to low sensitivity to aerosol absorption for longer channels at relatively low aerosol optical depths. The effect of applying the new version of smoothness constraints, termed relaxed, on retrievals of single-scattering albedo is analyzed for case studies of different aerosol types: black- and brown-carbon-containing fine mode aerosols, mineral dust coarse mode aerosols, and urban industrial fine mode aerosol. It is shown that for brown-carbon-containing aerosols employing the relaxed smoothness constraints resulted in significant reduction in retrieved single-scattering albedo and spectral residual errors (compared to standard) at the short wavelengths. For example, biomass burning smoke cases showed a reduction in single-scattering albedo and spectral residual error at 380 nm of ∼ 0.033 and ∼ 17 %, respectively, for the Rexburg site and ∼ 0.04 and ∼ 12.7 % for the Rimrock site, both AERONET sites in Idaho, USA. For a site with very high levels of black-carbon-containing aerosols (Mongu, Zambia), the effect of modification in the smoothness constraints was minor. For mineral dust aerosols at small Ångström exponent values (Mezaira site, UAE), the spectral constraint on the imaginary part of the refractive index was already relaxed in Version 3; therefore the new relaxed constraint results in minimal change. In the case of weakly absorbing urban industrial aerosols at the GSFC site, there are significant changes in retrieved single-scattering albedo using relaxed assumption, especially reductions at longer wavelengths: ∼ 0.016 and ∼ 0.02 at 875 and 1020 nm, respectively, for 440 nm aerosol optical depth (AOD) ∼ 0.3. The modification of smoothness constraints on the imaginary part of the refractive index has a minor effect on retrievals of other aerosol parameters such as the real part of the refractive index and parameters of the aerosol size distribution. The implementation of the relaxed smoothness constraints on the imaginary part of the refractive index in the next version of the AERONET inversion algorithm will produce significant impacts at some sites in short wavelength channels (380 and 440 nm) for some biomass burning smoke cases with significant brown carbon content and possibly in mid-visible channels (500 and 675 nm) to near-infrared channels (870 to 1020 nm) for some urban industrial aerosol types. However, most differences in single-scattering albedo retrievals between those applying the new relaxed constraint and the standard constraint will be within the uncertainty of the single-scattering albedo retrievals, depending on the level of aerosol optical depth, Ångström exponent, brown carbon content and wavelength.
Quantification of dust aerosols in Earth System Models (ESMs) has important implications for water cycle and biogeochemistry studies. This study examines the global life cycle and direct radiative effects (DREs) of dust in the U.S. Department of Energy's Energy Exascale Earth System Model version 1 (E3SMv1), and the impact of increasing model resolution both horizontally and vertically. The default 1° E3SMv1 captures the spatial and temporal variability in the observed dust aerosol optical depth (DAOD) reasonably well, but overpredicts dust absorption in the shortwave (SW). Simulations underestimate the dust vertical and long-range transport, compared with the satellite dust extinction profiles. After updating dust refractive indices and correcting for a bias in partitioning size-segregated emissions, both SW cooling and longwave (LW) warming of dust simulated by E3SMv1 are increased and agree better with other recent studies. The estimated net dust DRE of –0.42 Wm –2 represents a stronger cooling effect than the observationally based estimate –0.2 Wm –2 (–0.48 to +0.2), due to a smaller LW warming. Constrained by a global mean DAOD, model sensitivity studies of increasing horizontal and vertical resolution show strong influences on the simulated global dust burden and lifetime primarily through the change of dust dry deposition rate; there are also remarkable differences in simulated spatial distributions of DAOD, DRE, and deposition fluxes. Thus, constraining the global DAOD is insufficient for accurate representation of dust climate effects, especially in transitioning to higher- or variable-resolution ESMs. Better observational constraints of dust vertical profiles, dry deposition, size, and LW properties are needed.
Knowing the optical properties of aerosol dust is important for designing electro-optical systems and for modeling the effect on propagation of light in the atmosphere. As CO2 lidar technology becomes more advanced and is used for multiwavelength measurements, information on the wavelength dependent backscattering of aerosol dust particles is required. The volume backscattering coefficient of aerosols in the IR is relatively small. Thus, only a few field measurements of backscattering, usually at only a few wavelengths, are reported in the literature. We present spectral field measurements of backscattering of kaolin dust in the 9-11 micron wavelength range. As the quantity of dust increases, multiple scattering contributes more to the measured backscattered signal. The measurements show the effect of the dust quantity of the spectral backscatter measurements. A simple analytical two stream radiative transfer model is applied to confirm the measurements and to give insight to the multiple scattering spectra of backscattering.