Thomas Diehl

Global View of Aerosol Vertical Distributions from CALIPSO Lidar Measurements and GOCART Simulations: Regional and Seasonal Variations

This study examines seasonal variations of the vertical distribution of aerosols through a statistical analysis of the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) lidar observations from June 2006 to November 2007. A data-screening scheme is developed to attain good quality data in cloud-free conditions, and the polarization measurement is used to separate dust from non-dust aerosol. The CALIPSO aerosol observations are compared with aerosol simulations from the Goddard Chemistry Aerosol Radiation Transport (GOCART) model and aerosol optical depth (AOD) measurements from the MODerate resolution Imaging Spectroradiometer (MODIS). The CALIPSO observations of geographical patterns and seasonal variations of AOD are generally consistent with GOCART simulations and MODIS retrievals especially near source regions, while the magnitude of AOD shows large discrepancies in most regions. Both the CALIPSO observation and GOCART model show that the aerosol extinction scale heights in major dust and smoke source regions are generally higher than that in industrial pollution source regions. The CALIPSO aerosol lidar ratio also generally agrees with GOCART model within 30% on regional scales. Major differences between satellite observations and GOCART model are identified, including (1) an underestimate of aerosol extinction by GOCART over the Indian sub-continent, (2) much larger aerosol extinction calculated by GOCART than observed by CALIPSO in dust source regions, (3) much weaker in magnitude and more concentrated aerosol in the lower atmosphere in CALIPSO observation than GOCART model over transported areas in midlatitudes, and (4) consistently lower aerosol scale height by CALIPSO observation than GOCART model. Possible factors contributing to these differences are discussed.

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.

A satellite-based assessment of transpacific transport of pollution aerosol

[1] It has been well documented that pollution and dust from east Asia can be transported across the North Pacific basin, reaching North America and beyond. In this study, we assess the transpacific transport of ‘‘pollution aerosol’’ (defined as a mixture of aerosols from urban/industrial pollution and biomass burning) by taking advantage of the much improved measurement accuracy and enhanced new capabilities of satellite sensors in recent years. A 4-year (2002 to 2005) climatology of optical depth for pollution aerosol was generated from Moderate Resolution Imaging Spectroradiometer (MODIS) observations of fine- and coarse-mode aerosol optical depths. The pollution aerosol mass loading and fluxes were then calculated using measurements of the dependence of aerosol mass extinction efficiency on relative humidity and of aerosol vertical distributions from field campaigns and available satellite observations in the region. We estimated that about 18 Tg/a pollution aerosol is exported from east Asia to the northwestern Pacific Ocean, of which about 25% reaches the west coast of North America. The imported flux of 4.4 Tg/a to North America is equivalent to about 15% of local emissions from the United States and Canada. The pollution fluxes are largest in spring and smallest in summer. For the period we have examined the strongest export and import of pollution particulates occurred in 2003, largely because of record intense Eurasia boreal forest fires in spring and summer. The overall uncertainty of pollution fluxes is estimated at a factor of 2. Simulations by the Goddard Chemistry Aerosol Radiation and Transport (GOCART) and Global Modeling Initiative (GMI) models agree quite well with the satellite-based estimates of annual and latitude-integrated fluxes, with larger model-satellite differences in latitudinal and seasonal variations of fluxes.

Variability of marine aerosol fine-mode fraction and estimates of anthropogenic aerosol component over cloud-free oceans from the Moderate Resolution Imaging Spectroradiometer (MODIS)

[1]In this study, we examine seasonal and geographical variability of marine aerosol fine-mode fraction (f m ) and its impacts on deriving the anthropogenic component of aerosol optical depth (t a ) and direct radiative forcing from multispectral satellite measurements. A proxy off m , empirically derived from the Moderate Resolution Imaging Spectroradiometer (MODIS) Collection 5 data, shows large seasonal and geographical variations that are consistent with the Goddard Chemistry Aerosol Radiation Transport (GOCART) and Global Modeling Initiative (GMI) model simulations. The so-derived seasonally and spatially varyingf m is then implemented into a method of estimatingt a and direct radiative forcing from the MODIS measurements. It is found that the use of a constant value forf m as in previous studies would have overestimatedt a by about 20% over global ocean, with the overestimation up to!45% in some regions and seasons. The 7-year (2001‐2007) global ocean averaget a is 0.035, with yearly average ranging from 0.031 to 0.039. Future improvement in measurements is needed to better separate anthropogenic aerosol from natural ones and to narrow down the wide range of aerosol direct radiative forcing.

A multi‐model study of the hemispheric transport and deposition of oxidised nitrogen

Fifteen chemistry-transport models are used to quantify, for the first time, the export of oxidised nitrogen (NOy) to and from four regions (Europe, North America, South Asia, and East Asia), and to estimate the uncertainty in the results. Between 12 and 24% of the NOx emitted is exported from each region annually. The strongest impact of each source region on a foreign region is: Europe on East Asia, North America on Europe, South Asia on East Asia, and East Asia on North America. Europe exports the most NOy, and East Asia the least. East Asia receives the most NOy from the other regions. Between 8 and 15% of NOx emitted in each region is transported over distances larger than 1000 km, with 3–10% ultimately deposited over the foreign regions.

Sources, sinks, and transatlantic transport of North African dust aerosol: A multimodel analysis and comparison with remote sensing data

This study evaluates model-simulated dust aerosols over North Africa and the North Atlantic from five global models that participated in the Aerosol Comparison between Observations and Models phase II model experiments. The model results are compared with satellite aerosol optical depth (AOD) data from Moderate Resolution Imaging Spectroradiometer (MODIS), Multiangle Imaging Spectroradiometer (MISR), and Sea-viewing Wide Field-of-view Sensor, dust optical depth (DOD) derived from MODIS and MISR, AOD and coarse-mode AOD (as a proxy of DOD) from ground-based Aerosol Robotic Network Sun photometer measurements, and dust vertical distributions/centroid height from Cloud Aerosol Lidar with Orthogonal Polarization and Atmospheric Infrared Sounder satellite AOD retrievals. We examine the following quantities of AOD and DOD: (1) the magnitudes over land and over ocean in our study domain, (2) the longitudinal gradient from the dust source region over North Africa to the western North Atlantic, (3) seasonal variations at different locations, and (4) the dust vertical profile shape and the AOD centroid height (altitude above or below which half of the AOD is located). The different satellite data show consistent features in most of these aspects; however, the models display large diversity in all of them, with significant differences among the models and between models and observations. By examining dust emission, removal, and mass extinction efficiency in the five models, we also find remarkable differences among the models that all contribute to the discrepancies of model-simulated dust amount and distribution. This study highlights the challenges in simulating the dust physical and optical processes, even in the best known dust environment, and stresses the need for observable quantities to constrain the model processes.

The Interactive Stratospheric Aerosol Model Intercomparison Project (ISA-MIP): Motivation and experimental design

The Stratospheric Sulfur and its Role in Climate (SSiRC) Interactive Stratospheric Aerosol Model Intercomparison Project (ISA-MIP) explores uncertainties in the processes that connect volcanic emission of sulfur gas species and the radiative forcing associated with the resulting enhancement of the stratospheric aerosol layer. The central aim of ISA-MIP is to constrain and improve interactive stratospheric aerosol models and reduce uncertainties in the stratospheric aerosol forcing by comparing results of standardized model experiments with a range of observations. In this paper we present four co-ordinated inter-model experiments designed to investigate key processes which influence the formation and temporal development of stratospheric aerosol in different time periods of the observational record. The Background (BG) experiment will focus on microphysics and transport processes under volcanically quiescent conditions, when the stratospheric aerosol is controlled by the transport of aerosols and their precursors from the troposphere to the stratosphere. The Transient Aerosol Record (TAR) experiment will explore the role of smallto moderate-magnitude volcanic eruptions, anthropogenic sulfur emissions, and transport processes over the period 1998– 2012 and their role in the warming hiatus. Two further experiments will investigate the stratospheric sulfate aerosol evolution after major volcanic eruptions. The Historical Eruptions SO2 Emission Assessment (HErSEA) experiment will focus on the uncertainty in the initial emission of recent large-magnitude volcanic eruptions, while the Pinatubo EmPublished by Copernicus Publications on behalf of the European Geosciences Union. 2582 C. Timmreck et al.: ISA-MIP: motivation and experimental design ulation in Multiple models (PoEMS) experiment will provide a comprehensive uncertainty analysis of the radiative forcing from the 1991 Mt Pinatubo eruption.

Aerosols in the Atmosphere: Sources, Transport, and Multi-decadal Trends

We present our recent studies with global modeling and analysis of atmospheric aerosols. We have used the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model and satellite and in situ data to investigate (1) long-term variations of aerosols over polluted and dust source regions and downwind ocean areas in the past three decades and the cause of the changes and (2) anthropogenic and volcanic contributions to the sulfate aerosol in the upper troposphere/lower stratosphere.

Connection Between East Asian Air Pollution and Monsoon System

We present in this chapter a study on connections between the wintertime East Asian air pollution phenomenon and the monsoon strength. East Asia has been experiencing a fast worsening of air quality in recent years, particularly in winter, a problem commonly attributed to the increase of pollutant emissions associated with the rapid economic development. Meanwhile, previous studies have shown that the decadal-scale weakening of the Asian monsoon also contributed to the increase of PM2.5 (particulate matter with diameter less than 2.5 μm), a major pollutant that determines the air quality. Using a global modeling system, we investigate the emission and meteorological effects on the wintertime surface PM2.5 concentrations in East Asia in the past 30 years and find their relationship to the monsoon strength. We also examine the feedbacks between aerosols and meteorological fields via aerosol-radiation interaction to estimate the effects of such interaction on air quality.

Evaluation of the tropospheric chemistry general circulation model ECHAM5-MOZ and its application to the analysis of the chemical composition of the troposphere with an emphasis on the late RETRO period 1990-2000

The Tropospheric Chemistry General Circulation model ECHAM5-MOZ was developed between 2001 and 2005 and was used to investigate the variability and trends of ozone, CO and NOx in the second half of the 20th century in the framework of the RETRO project. The multi–decadal simulation of the period of 1960 to 2000 was one of the first of that kind. The model captures many features of the seasonal cycle and vertical gradients of trace gas concentrations measured on the ground or from balloons, aircraft or satellite. We diagnose a significant high bias in the simulated ozone concentrations in the 1990s, which can in part be attributed to an overestimated stratosphere troposphere exchange and possibly underestimated dry deposition of ozone. Wintertime CO concentrations in the northern hemisphere are underestimated by up to 30%. The observed interannual variability of the tropospheric NO2 column, surface CO concentrations and ozone is generally captured by the simulation, but the model fails to capture the surface ozone increase observed at several stations around the world during the 1980s and 1990s. The increase in the tropospheric ozone column between the 1960s and 1990s is consistent with model simulations of preindustrial conditions. The global ozone burden and chemical formation and loss are continuously rising during the entire 41-year simulation period. The dry deposition flux increases until the early 1980s and shows a more irregular behavior afterwards. Until around 1980 regionally averaged precursor emissions correlate well with surface ozone changes. Thereafter, the emission trend in Europe and North America is reversed, while ozone levels remain high. Asian emissions and ozone concentrations continue to rise, but the slope of the correlation changes.