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Contribution of mixing to upward transport across the tropical tropopause layer (TTL)

During the second part of the TROCCINOX campaign that took place in Brazil in early 2005, chemical species were measured on-board the high-altitude research aircraft Geophysica (ozone, water vapor, NO, NOy, CH4 and CO) in the altitude range up to 20 km (or up to 450 K potential temperature), i.e. spanning the entire TTL region roughly extending between 350 and 420 K. Here, analysis of transport across the TTL is performed using a new version of the Chemical Lagrangian Model of the Stratosphere (CLaMS). In this new version, the stratospheric model has been extended to the earth surface. Above the tropopause, the isentropic and cross-isentropic advection in CLaMS is driven by meteorological analysis winds and heating/cooling rates derived from a radiation calculation. Below the tropopause, the model smoothly transforms from the isentropic to the hybrid-pressure coordinate and, in this way, takes into account the effect of large-scale convective transport as implemented in the vertical wind of the meteorological analysis. As in previous CLaMS simulations, the irreversible transport, i.e. mixing, is controlled by the local horizontal strain and vertical shear rates. Stratospheric and tropospheric signatures in the TTL can be seen both in the observations and in the model. The composition of air above ≈350 K is mainly controlled by mixing on a time scale of weeks or even months. Based on CLaMS transport studies where mixing can be completely switched off, we deduce that vertical mixing, mainly driven by the vertical shear in the tropical flanks of the subtropical jets and, to some extent, in the the outflow regions of the large-scale convection, offers an explanation for the upward transport of trace species from the main convective outflow at around 350 K up to the tropical tropopause around 380 K.
Global trends in visibility: implications for dust sources

There is a large uncertainty in the relative roles of human land use, climate change and carbon dioxide fertilization in changing desert dust source strength over the past 100 years, and the overall sign of human impacts on dust is not known. We used visibility data from meteorological stations in dusty regions to assess the anthropogenic impact on long term trends in desert dust emissions. We did this by looking at time series of visibility derived variables and their correlations with precipitation, drought, winds, land use and grazing. Visibility data are available at thousands of stations globally from 1900 to the present, but we focused on 357 stations with more than 30 years of data in regions where mineral aerosols play a dominant role in visibility observations. We evaluated the 1974 to 2003 time period because most of these stations have reliable records only during this time. We first evaluated the visibility data against AERONET aerosol optical depth data, and found that only in dusty regions are the two moderately correlated. Correlation coefficients between visibility-derived variables and AERONET optical depths indicate a moderate correlation (0.47), consistent with capturing about 20% of the variability in optical depths. Two visibility-derived variables appear to compare the best with AERONET observations: the fraction of observations with visibility less than 5 km (VIS5) and the surface extinction (EXT). Regional trends show that in many dusty places, VIS5 and EXT are statistically significantly correlated with the Palmer drought severity index (based on precipitation and temperature) or surface wind speeds, consistent with dust temporal variability being largely driven by meteorology. This is especially true for North African and Chinese dust sources, but less true in the Middle East, Australia or South America, where there are not consistent patterns in the correlations. Climate indices such as El Nino or the North Atlantic Oscillation are not correlated with visibility-derived variables in this analysis. There are few stations where visibility measures are correlated with cultivation or grazing estimates on a temporal basis, although this may be a function of the very coarse temporal resolution of the land use datasets. On the other hand, spatial analysis of the visibility data suggests that natural topographic lows are not correlated with VIS5 or EXT, but land use is correlated at a moderate level. This analysis is consistent with land use being important in some regions, but meteorology driving interannual variability during 1974–2003.
Global statistics of liquid water content and effective number concentration of water clouds over ocean derived from combined CALIPSO and MODIS measurements

This study presents an empirical relation that links the volume extinction coefficients of water clouds, the layer integrated depolarization ratios measured by lidar, and the effective radii of water clouds derived from collocated passive sensor observations. Based on Monte Carlo simulations of CALIPSO lidar observations, this method combines the cloud effective radius reported by MODIS with the lidar depolarization ratios measured by CALIPSO to estimate both the liquid water content and the effective number concentration of water clouds. The method is applied to collocated CALIPSO and MODIS measurements obtained during July and October of 2006, and January 2007. Global statistics of the cloud liquid water content and effective number concentration are presented.
Hydrocarbon fluxes above a Scots pine forest canopy: measurements and modeling

We measured the fluxes of several hydrocarbon species above a Scots pine (Pinus sylvestris) stand using disjunct eddy covariance technique with proton transfer reaction – mass spectrometry. The measurements were conducted during four days in July at SMEAR II research station in Hyytiälä, Finland. Compounds which showed significant emission fluxes were methanol, acetaldehyde, acetone, and monoterpenes. A stochastic Lagrangian transport model with simple chemical degradation was applied to assess the sensitivity of the above canopy fluxes to chemistry. According to the model, the chemical degradation had a minor effect on the fluxes measured in this study but may have a major effect on the vertical flux profiles of more reactive compounds, such as sesquiterpenes. The monoterpene fluxes derived using M81 and M137 had a systematic difference with the latter one being higher. These fluxes followed the traditional exponential temperature dependent emission algorithm but were considerably higher than the fluxes measured before at the same site. The normalized monoterpene emission potentials at 30°C, obtained using the temperature dependence coefficient of 0.09°C−1, were 2.0 μg gdw−1 h−1 and 2.5 μg gdw−1 h−1, for fluxes derived using M81 and M137.
In-situ observations and modeling of small nitric acid-containing ice crystals

Measurements in nascent ice forming regions are very rare and help understand cirrus cloud formation and the interactions of trace gases with ice crystals. A tenuous cirrus cloud has been probed with in-situ and remote sensing instruments onboard the high altitude research aircraft Geophysica M55 in the tropical upper troposphere. Besides microphysical and optical particle properties, water (H2O) and reactive nitrogen species (NOy) have been measured. In slightly ice supersaturated air between 14.2 and 14.9 km altitude, an unusually low ice water content of 0.031 mg m−3 and small ice crystals with mean radii of 5 µm have been detected. A high nitric acid to water molar ratio (HNO3/H2O) of 5.4×10−5 has been observed in the ice crystals, about an order of magnitude higher compared to previous observations in cirrus at temperatures near 202 K. A model describing the trapping of HNO3 in growing ice particles shows that a high HNO3 content in ice crystals is expected during early growth stages, mainly originating from uptake in aerosol particles prior to freezing. Water vapor deposition on ice crystals and trapping of additional HNO3 reduces the molar ratio to values close to the ratio of HNO3/H2O in the gas phase while the cloud ages.
Physical and optical aerosol properties at the Dutch North Sea coast based on AERONET observations

Sun photometer measurements at the AERONET station at the North Sea coast in The Hague (The Netherlands) provide a climatology of optical and physical aerosol properties for the area. Results are presented from the period January 2002 to July 2003. For the analysis and interpretation these data are coupled to chemical aerosol data from a nearby station of the Dutch National Air Quality Network. This network provides PM10 and black carbon concentrations. Meteorological conditions and air mass trajectories are also used. Due to the location close to the coast, the results are strongly dependent on wind direction, i.e. air mass trajectory. In general the aerosol optical properties are governed by industrial aerosol emitted form various industrial, agricultural and urban areas surrounding the site in almost all directions over land. For maritime air masses industrial aerosols are transported from over the North Sea, whereas very clean air is transported from the NW in clean polar air masses from the North Atlantic. In the winter the effect of the production of sea salt aerosol at high wind speeds is visible in the optical and physical aerosol data. In these cases fine and coarse mode radii are similar to those reported in the literature for marine aerosol. Relations are derived between the Ångström coefficients with both the fine/coarse mode fraction and the ratio of black carbon and PM10.
A semi-analytical method for calculating rates of new sulfate aerosol formation from the gas phase

The formation of new aerosol from the gas phase is commonly represented in atmospheric modeling with parameterizations of the steady state nucleation rate. Present parameterizations are based on classical nucleation theory or on nucleation rates calculated with a numerical aerosol model. These parameterizations reproduce aerosol nucleation rates calculated with a numerical aerosol model only imprecisely. Additional errors can arise when the nucleation rate is used as a surrogate for the production rate of particles of a given size. We discuss these errors and present a method which allows a more precise calculation of steady state sulfate aerosol formation rates. The method is based on the semi-analytical solution of an aerosol system in steady state and on parameterized rate coefficients for H2SO4 uptake and loss by sulfate aerosol particles, calculated from laboratory and theoretical thermodynamic data.
Evaluation of ECMWF ERA-40 temperature and wind in the lower tropical stratosphere since 1988 from past long-duration balloon measurements

The temperature and wind of the ECMWF ERA-40 reanalysis in the tropical lower stratosphere during the period 1988–2001 has been evaluated by comparison with independent in situ measurements of 21 IR Montgolfier and superpressure long-duration balloon flights performed by CNES from Pretoria (26° S) in South Africa in 1988–1989, Latacunga (1° S) in Ecuador in 1991–1998 and Bauru (22° S) in Brazil in 2000–2001. The ERA-40 temperature displays a bias varying progressively from +1.16 K in 1988–1989, to +0.26 K in 1994–1996 and −0.46 K after 1998, the latter being fully consistent with recent evaluations of ECMWF operational analysis from radio occultation and in situ long-duration balloon observations. The amplitude of the bias and its evolution are very similar to the results of a previous evaluation from radiosondes in 1991–2003, suggesting that the origin of the drift of ERA-40 might be mainly due to errors in the series of satellite measurements of MSU, replaced by AMSU in 1998, assimilated in the model. The ERA-40 zonal wind speed in the lower stratosphere appears slightly overestimated by 0.7–1.0 m/s on average in both the tropics and equatorial region, that is by 5–10% compared to the average 10–20 m/s wind speed. This bias, fully consistent with a recent evaluation of ECMWF operational analysis in 2004, is found constant during the whole 1988–2001 period, suggesting a shortfall in the variabililty of ERA-40 horizontal winds in the lower stratosphere in the tropics and the equatorial region. Finally calculated trajectories using ERA-40, frequently used for analysing field observations, are found in error compared to that of the balloons by ±500 km after 5 days and ±1000 km after 10 days.
Including the sub-grid scale plume rise of vegetation fires in low resolution atmospheric transport models

We describe and begin to evaluate a parameterization to include the vertical transport of hot gases and particles emitted from biomass burning in low resolution atmospheric-chemistry transport models. This sub-grid transport mechanism is simulated by embedding a 1-D cloud-resolving model with appropriate lower boundary conditions in each column of the 3-D host model. Through assimilation of remote sensing fire products, we recognize which columns have fires. Using a land use dataset appropriate fire properties are selected. The host model provides the environmental conditions, allowing the plume rise to be simulated explicitly. The derived height of the plume is then used in the source emission field of the host model to determine the effective injection height, releasing the material emitted during the flaming phase at this height. Model results are compared with CO aircraft profiles from an Amazon basin field campaign and with satellite data, showing the huge impact that this mechanism has on model performance. We also show the relative role of each main vertical transport mechanisms, shallow and deep moist convection and the pyro-convection (dry or moist) induced by vegetation fires, on the distribution of biomass burning CO emissions in the troposphere.
Cloud microphysics and aerosol indirect effects in the global climate model ECHAM5-HAM

The double-moment cloud microphysics scheme from ECHAM4 that predicts both the mass mixing ratios and number concentrations of cloud droplets and ice crystals has been coupled to the size-resolved aerosol scheme ECHAM5-HAM. ECHAM5-HAM predicts the aerosol mass, number concentrations and mixing state. The simulated liquid, ice and total water content and the cloud droplet and ice crystal number concentrations as a function of temperature in stratiform mixed-phase clouds between 0 and −35° C agree much better with aircraft observations in the ECHAM5 simulations. ECHAM5 performs better because more realistic aerosol concentrations are available for cloud droplet nucleation and because the Bergeron-Findeisen process is parameterized as being more efficient. The total anthropogenic aerosol effect includes the direct, semi-direct and indirect effects and is defined as the difference in the top-of-the-atmosphere net radiation between present-day and pre-industrial times. It amounts to −1.9 W m−2 in ECHAM5, when a relative humidity dependent cloud cover scheme and aerosol emissions representative for the years 1750 and 2000 from the AeroCom emission inventory are used. The contribution of the cloud albedo effect amounts to −0.7 W m−2. The total anthropogenic aerosol effect is larger when either a statistical cloud cover scheme or a different aerosol emission inventory are employed because the cloud lifetime effect increases.