Yves Balkanski

Dust sources and deposition during the last glacial maximum and current climate: A comparison of model results with paleodata from ice cores and marine sediments

Mineral dust aerosols in the atmosphere have the potential to affect the global climate by influencing the radiative balance of the atmosphere and the supply of micronutrients to the ocean. Ice and marine sediment cores indicate that dust deposition from the atmosphere was at some locations 2–20 times greater during glacial periods, raising the possibility that mineral aerosols might have contributed to climate change on glacial-interglacial time scales. To address this question, we have used linked terrestrial biosphere, dust source, and atmospheric transport models to simulate the dust cycle in the atmosphere for current and last glacial maximum (LGM) climates. We obtain a 2.5-fold higher dust loading in the entire atmosphere and a twenty-fold higher loading in high latitudes, in LGM relative to present. Comparisons to a compilation of atmospheric dust deposition flux estimates for LGM and present in marine sediment and ice cores show that the simulated flux ratios are broadly in agreement with observations; differences suggest where further improvements in the simple dust model could be made. The simulated increase in high-latitude dustiness depends on the expansion of unvegetated areas, especially in the high latitudes and in central Asia, caused by a combination of increased aridity and low atmospheric [CO2]. The existence of these dust source areas at the LGM is supported by pollen data and loess distribution in the northern continents. These results point to a role for vegetation feedbacks, including climate effects and physiological effects of low [CO2], in modulating the atmospheric distribution of dust.

Three-dimensional climatological distribution of tropospheric OH: Update and evaluation

A global climatological distribution of tropospheric OH is computed using observed distributions of O3, H2O, NOt (NO2 +NO + 2N2O5 + NO3 + HNO2 +HNO4), CO, hydrocarbons, temperature, and cloud optical depth. Global annual mean OH is 1.16×106 molecules cm−3 (integrated with respect to mass of air up to 100 hPa within ±32° latitude and up to 200 hPa outside that region). Mean hemispheric concentrations of OH are nearly equal. While global mean OH increased by 33% compared to that from Spivakovsky et al. [1990], mean loss frequencies of CH3CCl3 and CH4 increased by only 23% because a lower fraction of total OH resides in the lower troposphere in the present distribution. The value for temperature used for determining lifetimes of hydrochlorofluorocarbons (HCFCs) by scaling rate constants [Prather and Spivakovsky, 1990] is revised from 277 K to 272 K. The present distribution of OH is consistent within a few percent with the current budgets of CH3CCl3 and HCFC-22. For CH3CCl3, it results in a lifetime of 4.6 years, including stratospheric and ocean sinks with atmospheric lifetimes of 43 and 80 years, respectively. For HCFC-22, the lifetime is 11.4 years, allowing for the stratospheric sink with an atmospheric lifetime of 229 years. Corrections suggested by observed levels of CH2Cl2 (annual means) depend strongly on the rate of interhemispheric mixing in the model. An increase in OH in the Northern Hemisphere by 20% combined with a decrease in the southern tropics by 25% is suggested if this rate is at its upper limit consistent with observations of CFCs and 85Kr. For the lower limit, observations of CH2Cl2 imply an increase in OH in the Northern Hemisphere by 35% combined with a decrease in OH in the southern tropics by 60%. However, such large corrections are inconsistent with observations for 14CO in the tropics and for the interhemispheric gradient of CH3CCl3. Industrial sources of CH2Cl2 are sufficient for balancing its budget. The available tests do not establish significant errors in OH except for a possible underestimate in winter in the northern and southern tropics by 15–20% and 10–15%, respectively, and an overestimate in southern extratropics by ∼25%. Observations of seasonal variations of CH3CCl3, CH2Cl2, 14CO, and C2H6 offer no evidence for higher levels of OH in the southern than in the northern extratropics. It is expected that in the next few years the latitudinal distribution and annual cycle of CH3CCl3 will be determined primarily by its loss frequency, allowing for additional constraints for OH on scales smaller than global.

Modeling the mineralogy of atmospheric dust sources

The variability of atmospheric dust mineralogy influences the impact of desert dust on the Earths radiative budget and biogeochemical cycles. Until now, atmospheric transport models have assumed that dust was a constant homogeneous mixture, hence neglecting this variability. The lack of mineralogical data in arid areas prevented a better description of the atmospheric dust composition, and we propose here a new formulation to estimate the mineral content of arid surfaces on a global scale. First, we collect a Database of Arid Soil Surface Mineralogy for eight major minerals: quartz, feldspar, calcite, gypsum, illite, kaolinite, smectite, and hematite, both for the clay and silt fraction. On the basis of this, we formulate a Mean Mineralogical Table that relates classical soil types to surface mineralogy. We use this table and the geographical distribution of soil types given in the Food and Agriculture Organization Soil Map of the World to obtain the mineralogy of arid surfaces globally. In order to validate these results, we present a compilation of measured mineralogical composition of dust samples with identified sources. The correlation between observed dust mineralogy and those inferred from soil types in corresponding areas is between 0.70 and 0.94. We then calculate the maps of the single scattering albedo and of the ratio of infrared extinction to visible extinction for the erodible fraction of arid areas. Mineralogical maps presented here will be used in future studies with an emission scheme in a global transport model.

Transport and residence times of tropospheric aerosols inferred from a global three‐dimensional simulation of 210Pb

A global three-dimensional model is used to investigate the transport and tropospheric residence time of 210Pb, an aerosol tracer produced in the atmosphere by radioactive decay of 222Rn emitted from soils. The model uses meteorological input with 4°×5° horizontal resolution and 4-hour temporal resolution from the Goddard Institute for Space Studies general circulation model (GCM). It computes aerosol scavenging by convective precipitation as part of the wet convective mass transport operator in order to capture the coupling between vertical transport and rainout. Scavenging in convective precipitation accounts for 74% of the global 210Pb sink in the model; scavenging in large-scale precipitation accounts for 12%, and scavenging in dry deposition accounts for 14%. The model captures 63% of the variance of yearly mean 210Pb concentrations measured at 85 sites around the world with negligible mean bias, lending support to the computation of aerosol scavenging. There are, however, a number of regional and seasonal discrepancies that reflect in part anomalies in GCM precipitation. Computed residence times with respect to deposition for 210Pb aerosol in the tropospheric column are about 5 days at southern midlatitudes and 10–15 days in the tropics; values at northern midlatitudes vary from about 5 days in winter to 10 days in summer. The residence time of 210Pb produced in the lowest 0.5 km of atmosphere is on average four times shorter than that of 210Pb produced in the upper atmosphere. Both model and observations indicate a weaker decrease of 210Pb concentrations between the continental mixed layer and the free troposphere than is observed for total aerosol concentrations; an explanation is that 222Rn is transported to high altitudes in wet convective updrafts, while aerosols and soluble precursors of aerosols are scavenged by precipitation in the updrafts. Thus 210Pb is not simply a tracer of aerosols produced in the continental boundary layer, but also of aerosols derived from insoluble precursors emitted from the surface of continents. One may draw an analogy between 210Pb and nitrate, whose precursor NOx is sparingly soluble, and explain in this manner the strong correlation observed between nitrate and 210Pb concentrations over the oceans.

Evaluation and intercomparison of global atmospheric transport models using 222Rn and other short‐lived tracers

Simulations of 222Rn and other short-lived tracers are used to evaluate and intercompare the representations of convective and synoptic processes in 20 global atmospheric transport models. Results show that most established three-dimensional models simulate vertical mixing in the troposphere to within the constraints offered by the observed mean 222Rn concentrations and that subgrid parameterization of convection is essential for this purpose. However, none of the models captures the observed variability of 222Rn concentrations in the upper troposphere, and none reproduces the high 222Rn concentrations measured at 200 hPa over Hawaii. The established three-dimensional models reproduce the frequency and magnitude of high-222Rn episodes observed at Crozet Island in the Indian Ocean, demonstrating that they can resolve the synoptic-scale transport of continental plumes with no significant numerical diffusion. Large differences between models are found in the rates of meridional transport in the upper troposphere (interhemispheric exchange, exchange between tropics and high latitudes). The four two-dimensional models which participated in the intercomparison tend to underestimate the rate of vertical transport from the lower to the upper troposphere but show concentrations of 222Rn in the lower troposphere that are comparable to the zonal mean values in the three-dimensional models.

Uncertainties in assessing radiative forcing by mineral dust

The assessment of the climatic effects of an aerosol with a large variability like mineral dust requires some approximations whose validity is investigated in this paper. Calculations of direct radiative forcing by mineral dust (short-wave, long-wave and net) are performed with a single-column radiation model for two standard cases in clear sky condition: a desert case and an oceanic case. Surface forcing result from a large diminution of the short-wave fluxes and of the increase in down-welling long-wave fluxes. Top of the atmosphere (TOA) forcing is negative when short-wave backscattering dominates, for instance above the ocean, and positive when short-wave or long-wave absorption dominates, which occurs above deserts. We study here the sensitivity of these mineral forcings to different treatments of the aerosol complex refractive index and size distribution. We also describe the importance of the dust vertical profile, ground temperature, emissivity and albedo. Among these parameters, the aerosol complex refractive index has been identified as a critical parameter given the paucity and the incertitude associated with it. Furthermore, the imaginary part of the refractive index is inadequate if spectrally averaged. Its natural variability (linked to mineralogical characteristics) lead to variations of up to ±40% in aerosol forcing calculations. A proper representation of the size distribution when modelling mineral aerosols is required since dust optical properties are very sensitive to the presence of small particles. In addition we demonstrate that LW forcing imply a non-negligible sensitivity to the vertical profiles of temperature and dust, the latter being an important constraint for dust effect calculations.

Role of aerosol size distribution and source location in a three‐dimensional simulation of a Saharan dust episode tested against satellite‐derived optical thickness

An off-line global three-dimensional tracer model based on analyzed wind fields was augmented to simulate the atmospheric transport of mineral dust. The model describes the evolution of the aerosol size distribution and hence allows to compute aerosol number and mass concentrations. In this study we describe the parameterization of the sedimentation process and include a preliminary source formulation but exclude wet deposition. Validation of the model is done during a 16-day period in June-July 1988 with very scarce precipitation. It is based on a comparison of every model grid box with daily satellite-derived optical thickness observations of Saharan dust plumes over the North Atlantic and the Mediterranean. The model reproduces accurately the daily position of the dust plumes over the ocean, with the exception of Atlantic regions remote from the African coast. By systematic analysis of transport and aerosol components we show that the largest uncertainty in reproducing the position of the dust clouds is the correct localization of the source regions. The model simulation is also very sensitive to the inclusion of convection and to an accurate treatment of the sedimentation process. Only the combination of source activation, rapid transport of dust to higher altitudes by convective updraft and long-range transport allows the simulation of the dust plumes position. This study shows that a mineral dust transport model is only constrained if both the source strength and the aerosol size distribution are known. The satellite observation of optical thickness over the Mediterranean and assumptions about the size distribution indicate that the dust emission flux was of the order of 17×106 t for the 16-day period under investigation. The simulations suggest that a major aerosol mode initially around 2.5 μm with a standard deviation of 2.0 plays the dominant role in long-range transport of mineral dust.

Seasonal and interannual variability of the mineral dust cycle under present and glacial climate conditions

[1] We present simulations of the dust cycle during present and glacial climate states, using a model, which explicitly simulates the control of dust emissions as a function of seasonal and interannual changes in vegetation cover. The model produces lower absolute amounts of dust emissions and deposition than previous simulations of the Last Glacial Maximum (LGM) dust cycle. However, the simulated 2- to 3-fold increase in emissions and deposition at the LGM compared to today, is in agreement with marine- and ice-core observations, and consistent with previous simulations. The mean changes are accompanied by a prolongation of the length of the season of dust emissions in most source regions. The increase is most pronounced in Asia, where LGM dust emissions are high throughout the winter, spring and summer rather than occurring primarily in spring as they do today. Changes in the seasonality of dust emissions, and hence atmospheric loading, interact with changes in the seasonality of precipitation, and hence of the relative importance of wet and dry deposition processes at high northern latitudes. As a result, simulated dust deposition rates in the high northern latitudes show high interannual variability. Our results suggest that the high dust concentration variability shown by the Greenland ice core records during the LGM is a consequence of changes in atmospheric circulation and precipitation locally rather than a result of changes in the variability of dust emissions. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0315 Atmospheric Composition and Structure: Biosphere/atmosphere interactions; 1615 Global Change: Biogeochemical processes (4805); 3319 Meteorology and Atmospheric Dynamics: General circulation; 3344 Meteorology and Atmospheric Dynamics: Paleoclimatology; KEYWORDS: dust, mineral aerosol, glacial climate, GCM simulation, LGM, GRIP/GISP ice cores

Application of the CALIOP layer product to evaluate the vertical distribution of aerosols estimated by global models: AeroCom phase i results

[1] The CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) layer product is used for a multimodel evaluation of the vertical distribution of aerosols. Annual and seasonal aerosol extinction profiles are analyzed over 13 sub-continental regions representative of industrial, dust, and biomass burning pollution, from CALIOP 2007–2009 observations and from AeroCom (Aerosol Comparisons between Observations and Models) 2000 simulations. An extinction mean height diagnostic (Za) is defined to quantitatively assess the models’ performance. It is calculated over the 0–6 km and 0–10 km altitude ranges by weighting the altitude of each 100 m altitude layer by its aerosol extinction coefficient. The mean extinction profiles derived from CALIOP layer products provide consistent regional and seasonal specificities and a low inter-annual variability. While the outputs from most models are significantly correlated with the observed Za climatologies, some do better than others, and 2 of the 12 models perform particularly well in all seasons. Over industrial and maritime regions, most models show higher Za than observed by CALIOP, whereas over the African and Chinese dust source regions, Za is underestimated during Northern Hemisphere Spring and Summer. The positive model bias in Za is mainly due to an overestimate of the extinction above 6 km. Potential CALIOP and model limitations, and methodological factors that might contribute to the differences are discussed.

Estimates of global multicomponent aerosol optical depth and direct radiative perturbation in the Laboratoire de Météorologie Dynamique general circulation model

(1) The global cycle of multicomponent aerosols including sulfate, black carbon (BC), organic matter (OM), mineral dust, and sea salt is simulated in the Laboratoire de Meteorologie Dynamique general circulation model (LMDZT GCM). The seasonal open biomass burning emissions for simulation years 2000-2001 are scaled from climatological emissions in proportion to satellite detected fire counts. The emissions of dust and sea salt are parameterized online in the model. The comparison of model-predicted monthly mean aerosol optical depth (AOD) at 500 nm with Aerosol Robotic Network (AERONET) shows good agreement with a correlation coefficient of 0.57(N = 1324) and 76% of data points falling within a factor of 2 deviation. The correlation coefficient for daily mean values drops to 0.49 (N = 23,680). The absorption AOD (ta at 670 nm) estimated in the model is poorly correlated with measurements (r = 0.27, N = 349). It is biased low by 24% as compared to AERONET. The model reproduces the prominent features in the monthly mean AOD retrievals from Moderate Resolution Imaging Spectroradiometer (MODIS). The agreement between the model and MODIS is better over source and outflow regions (i.e., within a factor of 2). There is an underestimation of the model by up to a factor of 3 to 5 over some remote oceans. The largest contribution to global annual average AOD (0.12 at 550 nm) is from sulfate (0.043 or 35%), followed by sea salt (0.027 or 23%), dust (0.026 or 22%), OM (0.021 or 17%), and BC (0.004 or 3%). The atmospheric aerosol absorption is predominantly contributed by BC and is about 3% of the total AOD. The globally and annually averaged shortwave (SW) direct aerosol radiative perturbation (DARP) in clear-sky conditions is � 2.17 Wm � 2 and is about a factor of 2 larger than in all-sky conditions (� 1.04 Wm � 2 ). The net DARP (SW + LW) by all aerosols is � 1.46 and � 0.59 Wm � 2 in clear- and all-sky conditions, respectively. Use of realistic, less absorbing in SW, optical properties for dust results in negative forcing over the dust-dominated regions.