We use a global chemical transport model (GEOS-Chem) to estimate the impact of transpacific transport of mineral dust on aerosol concentrations in North America during 2001. We have implemented two ...dust mobilization schemes in the model (GOCART and DEAD) and find that the best simulation of North American surface observations with GEOS-Chem is achieved by combining the topographic source used in GOCART with the entrainment scheme used in DEAD. This combination restricts dust emissions to year-round arid areas but includes a significant wind threshold for dust mobilization. The model captures the magnitude and seasonal cycle of observed surface dust concentrations over the northern Pacific. It simulates the free tropospheric outflow of dust from Asia observed in the TRACE-P and ACE-Asia aircraft campaigns of spring 2001. It reproduces the timing and distribution of Asian dust outbreaks in North America during April–May. Beyond these outbreaks we find persistent Asian fine dust (averaging 1.2
μg
m
−3) in surface air over the western United States in spring, with much weaker influence (0.25
μg
m
−3) in summer and fall. Asian influence over the eastern United States is 30–50% lower. We find that transpacific sources accounted for 41% of the worst dust days in the western United States in 2001.
Volcanic eruptions are important causes of natural variability in the climate system at all time scales. Assessments of the climate impact of volcanic eruptions by climate models almost universally ...assume that sulfate aerosol is the only radiatively active volcanic material. We report satellite observations from the Cloud‐Aerosol Lidar with Orthogonal Polarization (CALIOP) on board the Cloud‐Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite after the eruption of Mount Kelud (Indonesia) on 13 February 2014 of volcanic materials in the lower stratosphere. Using these observations along with in situ measurements with the Compact Optical Backscatter AerosoL Detector (COBALD) backscatter sondes and optical particle counters (OPCs) made during a balloon field campaign in northern Australia, we find that fine ash particles with a radius below 0.3 µm likely represented between 20 and 28% of the total volcanic cloud aerosol optical depth 3 months after the eruption. A separation of 1.5–2 km between the ash and sulfate plumes is observed in the CALIOP extinction profiles as well as in the aerosol number concentration measurements of the OPC after 3 months. The settling velocity of fine ash with a radius of 0.3 µm in the tropical lower stratosphere is reduced by 50% due to the upward motion of the Brewer‐Dobson circulation resulting a doubling of its lifetime. Three months after the eruption, we find a mean tropical clear‐sky radiative forcing at the top of the atmosphere from the Kelud plume near −0.08 W/m2 after including the presence of ash; a value ~20% higher than if sulfate alone is considered. Thus, surface cooling following volcanic eruptions could be affected by the persistence of ash and should be considered in climate simulations.
Key Points
In situ and spaceborne observations of the Kelud plume
Persistence of ash in the lower stratosphere
Ash can impact climate on longer time scale than previously thought
Interest in stratospheric aerosol and its role in climate have increased over the last decade due to the observed increase in stratospheric aerosol since 2000 and the potential for changes in the ...sulfur cycle induced by climate change. This review provides an overview about the advances in stratospheric aerosol research since the last comprehensive assessment of stratospheric aerosol was published in 2006. A crucial development since 2006 is the substantial improvement in the agreement between in situ and space-based inferences of stratospheric aerosol properties during volcanically quiescent periods. Furthermore, new measurement systems and techniques, both in situ and space based, have been developed for measuring physical aerosol properties with greater accuracy and for characterizing aerosol composition. However, these changes induce challenges to constructing a long-term stratospheric aerosol climatology. Currently, changes in stratospheric aerosol levels less than 20% cannot be confidently quantified. The volcanic signals tend to mask any nonvolcanically driven change, making them difficult to understand. While the role of carbonyl sulfide as a substantial and relatively constant source of stratospheric sulfur has been confirmed by new observations and model simulations, large uncertainties remain with respect to the contribution from anthropogenic sulfur dioxide emissions. New evidence has been provided that stratospheric aerosol can also contain small amounts of nonsulfatematter such as black carbon and organics. Chemistry-climate models have substantially increased in quantity and sophistication. In many models the implementation of stratospheric aerosol processes is coupled to radiation and/or stratospheric chemistry modules to account for relevant feedback processes.
We use satellite (MODIS) observations of aerosol optical depths (AODs) over the North Pacific, together with surface aerosol measurements at a network of remote U.S. sites (IMPROVE), to improve ...understanding of the transpacific transport of Asian aerosol pollution and assess the ability of a global 3‐D chemical transport model (GEOS‐Chem CTM) to quantify Asian aerosol enhancements in U.S. surface air. The MODIS observations show the strongest transpacific transport occurring in spring at 40–55°N. This transport in the model takes place mainly in the lower free troposphere (900–700 hPa) because of scavenging during transport either in the boundary layer or during lifting to the upper troposphere. The preferential altitude of aerosol transpacific transport results in direct impact on the elevated terrain of the NW United States. Sulfate observations in the NW United States in spring 2001 show higher concentrations on the days of model‐predicted maximum Asian influence (1.04 μg m−3) than seasonal mean values (0.69 μg m−3). No such Asian enhancements are observed for nitrate or for organic carbon (OC) aerosol. Distinct Asian sulfate episodes correlated with dust events are observed in the NW United States and simulated with the model. The mean Asian pollution enhancement in that region in spring is 0.16 μg m−3 with a 50% estimated uncertainty. This is higher than the estimated natural concentration of 0.09 μg m−3 presently used as objective for regulation of visibility in U.S. wilderness areas.
Global ozone analyses, based on assimilation of stratospheric profile and ozone column measurements, and NOy predictions from the Real‐time Air Quality Modeling System (RAQMS) are used to estimate ...the ozone and NOy budget over the continental United States during the July–August 2004 Intercontinental Chemical Transport Experiment–North America (INTEX‐A). Comparison with aircraft, satellite, surface, and ozonesonde measurements collected during INTEX‐A show that RAQMS captures the main features of the global and continental U.S. distribution of tropospheric ozone, carbon monoxide, and NOy with reasonable fidelity. Assimilation of stratospheric profile and column ozone measurements is shown to have a positive impact on the RAQMS upper tropospheric/lower stratosphere ozone analyses, particularly during the period when SAGE III limb scattering measurements were available. Eulerian ozone and NOy budgets during INTEX‐A show that the majority of the continental U.S. export occurs in the upper troposphere/lower stratosphere poleward of the tropopause break, a consequence of convergence of tropospheric and stratospheric air in this region. Continental U.S. photochemically produced ozone was found to be a minor component of the total ozone export, which was dominated by stratospheric ozone during INTEX‐A. The unusually low photochemical ozone export is attributed to anomalously cold surface temperatures during the latter half of the INTEX‐A mission, which resulted in net ozone loss during the first 2 weeks of August. Eulerian NOy budgets are shown to be very consistent with previously published estimates. The NOy export efficiency was estimated to be 24%, with NOx + PAN accounting for 54% of the total NOy export during INTEX‐A.
United Kingdom Meteorological Office global analyses from 1991 to 2001 are used to create a global climatology of stratospheric polar vortices and anticyclones. New methodologies are developed that ...identify vortices in terms of evolving three‐dimensional (3‐D) air masses. A case study illustrates the performance of the identification schemes during February and March of 1999 when a merger of anticyclones led to a stratospheric warming that split the Arctic polar vortex. The 3‐D structure and temporal evolution of the Arctic vortex and identified anticyclones demonstrates the algorithm's ability to capture complicated phenomena. The mean geographical distribution of polar vortex and anticyclone frequency is shown for each season. The frequency distributions illustrate the climatological location and persistence of polar vortices and anticyclones. A counterpart to the Aleutian High is documented in the Southern Hemisphere: the “Australian High.” The temporal evolution of the area occupied by polar vortices and anticyclones in each hemisphere is shown as a function of potential temperature. Large polar vortex area leads to an increase in anticyclone area, which in turn results in a decrease in the size of the polar vortex. During Northern winter and Southern spring, 9 years of daily anticyclone movement are shown on the 1200 K (36 km, 4 hPa) isentropic surface. Preferred locations of anticyclogenesis are related to cross‐equatorial flow and weak inertial stability. Regimes of traveling and stationary anticyclones are discussed.
The Asian Tropopause Aerosol Layer (ATAL) represents an accumulation of aerosol in the upper troposphere and lower stratosphere associated with the Asian Summer Monsoon. Here we simulate the ATAL for ...summer 2013 with the GEOS‐Chem chemical transport model and explore the likely composition of ATAL aerosols and the relative contributions of regional anthropogenic sources versus those from farther afield. The model indicates significant contributions from organic aerosol, nitrate, sulfate, and ammonium aerosol, with regional anthropogenic precursor sources dominant. The model underestimates aerosol backscatter in the ATAL during summer 2013, compared with Cloud‐Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite instrument. Tests of a more physically based treatment of wet scavenging of SO2 in convective updrafts raise sulfate, eliminating the low bias with respect to CALIPSO backscatter in the ATAL, but lead to an unacceptable high bias of sulfate compared with in situ observations from aircraft over the United States. Source apportionment of the model results indicate the dominance of regional anthropogenic emissions from China and the Indian subcontinent to aerosol concentrations in the ATAL; ~60% of sulfate in the ATAL region in August 2013 is attributable to anthropogenic sources of SO2 from China (~30%) and from the Indian subcontinent (~30%), twice as much as in previously published estimates. Nitrate aerosol is found to be a dominant component of aerosol composition on the southern flank of the Asian Summer Monsoon anticyclone. Lightning sources of NOx are found to make a significant (10–15%) contribution to nitrate in the ATAL for the case studied.
Key Points
Regional anthropogenic emissions from China and India dominate aerosol concentrations in the ATAL, in contrast with previous estimates
GEOS‐Chem underestimates aerosol backscatter in the ATAL during summer 2013, compared with CALIPSO satellite instrument
A more physically based treatment of wet scavenging of SO2 in convective updraft is tested in GEOS‐Chem
We use high‐frequency in situ observations made from the DC8 to examine fine‐scale tracer structure and correlations observed in the upper troposphere and lower stratosphere during INTEX‐NA. Two ...flights of the NASA DC‐8 are compared and contrasted. Chemical data from the DC‐8 flight on 18 July show evidence for interleaving and mixing of polluted and stratospheric air masses in the vicinity of the subtropical jet in the upper troposphere, while on 2 August the DC‐8 flew through a polluted upper troposphere and a lowermost stratosphere that showed evidence of an intrusion of polluted air. We compare data from both flights with RAQMS 3‐D global meteorological and chemical model fields to establish dynamical context and to diagnose processes regulating the degree of mixing on each day. We also use trajectory mapping of the model fields to show that filamentary structure due to upstream strain deformation contributes to tracer variability observed in the upper troposphere. An Eulerian measure of strain versus rotation in the large‐scale flow is found useful in predicting filamentary structure in the vicinity of the jet. Higher‐frequency (6–24 km) tracer variability is attributed to buoyancy wave oscillations in the vicinity of the jet, whose turbulent dissipation leads to efficient mixing across tracer gradients.
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