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Sensitivity of stratospheric inorganic chlorine to differences in transport

Correctly modeling stratospheric inorganic chlorine (Cly) is crucial for modeling the past and future evolution of stratospheric ozone. However, comparisons of the chemistry climate models used in the latest international assessment of stratospheric ozone depletion have shown large differences in the modeled Cly, with these differences explaining many of the differences in the simulated evolution of ozone over the next century. Here in, we examine the role of transport in determining the simulated Cly using three simulations from the same off-line chemical transport model that have the same lower tropospheric boundary conditions and the same chemical solver, but differing resolution and/or meteorological fields. These simulations show that transport plays a key role in determining the Cly distribution, and that Cly depends on both the time scales and pathways of transport. The time air spends in the stratosphere (e.g., the mean age) is an important transport factor determining stratospheric Cly, but the relationship between mean age and Cly is not simple. Lower stratospheric Cly depends on the fraction of air that has been in the upper stratosphere, and transport differences between models having the same mean age can result in differences in the fraction of organic chlorine converted into Cly. Differences in transport pathways result in differences in vertical profiles of CFCs, and comparisons of observed and modeled CFC profiles provide a stringent test of transport pathways in models.
A study of the effect of overshooting deep convection on the water content of the TTL and lower stratosphere from Cloud Resolving Model simulations

Simulations of overshooting, tropical deep convection using a Cloud Resolving Model with bulk microphysics are presented in order to examine the effect on the water content of the TTL (Tropical Tropopause Layer) and lower stratosphere. This case study is a subproject of the HIBISCUS (Impact of tropical convection on the upper troposphere and lower stratosphere at global scale) campaign, which took place in Bauru, Brazil (22° S, 49° W), from the end of January to early March 2004. Comparisons between 2-D and 3-D simulations suggest that the use of 3-D dynamics is vital in order to capture the mixing between the overshoot and the stratospheric air, which caused evaporation of ice and resulted in an overall moistening of the lower stratosphere. In contrast, a dehydrating effect was predicted by the 2-D simulation due to the extra time, allowed by the lack of mixing, for the ice transported to the region to precipitate out of the overshoot air. Three different strengths of convection are simulated in 3-D by applying successively lower heating rates (used to initiate the convection) in the boundary layer. Moistening is produced in all cases, indicating that convective vigour is not a factor in whether moistening or dehydration is produced by clouds that penetrate the tropopause, since the weakest case only just did so. An estimate of the moistening effect of these clouds on an air parcel traversing a convective region is made based on the domain mean simulated moistening and the frequency of convective events observed by the IPMet (Instituto de Pesquisas Meteorológicas, Universidade Estadual Paulista) radar (S-band type at 2.8 Ghz) to have the same 10 dBZ echo top height as those simulated. These suggest a fairly significant mean moistening of 0.26, 0.13 and 0.05 ppmv in the strongest, medium and weakest cases, respectively, for heights between 16 and 17 km. Since the cold point and WMO (World Meteorological Organization) tropopause in this region lies at ~15.9 km, this is likely to represent direct stratospheric moistening. Much more moistening is predicted for the 15–16 km height range with increases of 0.85–2.8 ppmv predicted. However, it would be required that this air is lofted through the tropopause via the Brewer Dobson circulation in order for it to have a stratospheric effect. Whether this is likely is uncertain and, in addition, the dehydration of air as it passes through the cold trap and the number of times that trajectories sample convective regions needs to be taken into account to gauge the overall stratospheric effect. Nevertheless, the results suggest a potentially significant role for convection in determining the stratospheric water content. Sensitivity tests exploring the impact of increased aerosol numbers in the boundary layer suggest that a corresponding rise in cloud droplet numbers at cloud base would increase the number concentrations of the ice crystals transported to the TTL, which had the effect of reducing the fall speeds of the ice and causing a ~13% rise in the mean vapour increase in both the 15–16 and 16–17 km height ranges, respectively, when compared to the control case. Increases in the total water were much larger, being 34% and 132% higher for the same height ranges, but it is unclear whether the extra ice will be able to evaporate before precipitating from the region. These results suggest a possible impact of natural and anthropogenic aerosols on how convective clouds affect stratospheric moisture levels.
The diurnal evolution of 222Rn and its progeny in the atmospheric boundary layer during the Wangara experiment

The diurnal atmospheric boundary layer evolution of the 222Rn decaying family is studied using a state-of-the-art large-eddy simulation model. In particular, a diurnal cycle observed during the Wangara experiment is successfully simulated together with the effect of diurnal varying turbulent characteristics on radioactive compounds initially in a secular equilibrium. This study allows us to clearly analyze and identify the boundary layer processes driving the behaviour of 222Rn and its progeny concentrations. An activity disequilibrium is observed in the nocturnal boundary layer due to the proximity of the radon source and the trapping of fresh 222Rn close to the surface induced by the weak vertical transport. During the morning transition, the secular equilibrium is fast restored by the vigorous turbulent mixing. The evolution of 222Rn and its progeny concentrations in the unsteady growing convective boundary layer depends on the strength of entrainment events.
Methane emissions from boreal and tropical forest ecosystems derived from in-situ measurements

Methane is a climatologically important greenhouse gas, which plays a key role in regulating water vapour in the stratosphere and hydroxyl radicals in the troposphere. Recent findings that vegetation emits methane have stimulated efforts to ascertain the impact of this source on the global budget. In this work, we present the results of high frequency (ca. 1 min−1) methane measurements conducted in the boreal forests of Finland and the tropical forests of Suriname, in April–May, 2005 and October 2005 respectively. The measurements were performed using a gas chromatograph – flame ionization detector (GC-FID). The average of the median mixing ratios during a typical diel cycle were 1.83 μmol mol−1 and 1.74 μmol mol−1 for the boreal forest ecosystem and tropical forest ecosystem respectively, with remarkable similarity in the time series of both the boreal and tropical diel profiles. Night time methane emission flux of the boreal forest ecosystem, calculated from the increase of methane during the night and measured nocturnal boundary layer heights yields a flux of (3.62±0.87)×1011 molecules cm−2 s−1(or 45.5±11 Tg CH4 yr−1 for global boreal forest area). This is a source contribution of circa 8% of the global methane budget. These results highlight the importance of the boreal and tropical forest ecosystems for the global budget of methane. The results are also discussed in the context of recent work reporting high methane mixing ratios over tropical forests using space borne near infra-red spectroscopy measurements.
Long-time global radiation for Central Europe derived from ISCCP Dx data

The global Dx dataset of the International Satellite Cloud Climatology Project (ISCCP) with a spatial resolution of about 30×30 km² was analysed to produce spatially highly resolved long-time datasets to describe the radiation budget for Central Europe over the period of 1984–2000. The computation of shortwave and longwave radiant flux densities at top of atmosphere and at surface was based on 1D radiative transfer simulations. The simulations were carried out for all relevant atmospheric and surface conditions and the results were inserted into a look-up table. Thus, long-time calculations for all conditions and time slices of the Dx dataset could be realised. The study is focussed on the global radiation at surface. The first examination was carried out for the ISCCP D1 and the ISCCP D2 dataset. These datasets, including cloud and surface information on a different spatial scale (280×280 km2), were applied to the produced look-up table analogue to the Dx data. The calculated global radiation of the D1 and D2 dataset were compared to the Dx dataset. The differences between these datasets mainly range from 5–15 Wm−2 (2–6%) with regional peaks up to 25 Wm−2 (10%). The evaluation with the GEWEX Surface Radiation Budget (SRB) data emphasises differences between 5–25 Wm−2 (6–16%) over land areas. Deviations to an ISCCP provided flux data set vary from 0 Wm−2 in the North up to 35 Wm−2 (0–13%) in the South of Central Europe. The global radiation datasets provided by the Global Energy Balance Archive (GEBA) and the German Meteorological Service (DWD) agree well, but they are 5–25 Wm−2 (7–10%) lower than the Dx results. Annual analyses of global radiation of various regional climate models complete the study. It is figured out that the used models and methods reveal a couple of discrepancies. Especially in wintertime the results of our analysis differ to the considered models. Principally the uncertainties were caused by the determined range of values and simplifications for the computation of the radiative transfer simulation.
Evaluation of ECMWF water vapour fields by airborne differential absorption lidar measurements: a case study between Brazil and Europe

Three extended airborne Differential Absorption Lidar (DIAL) sections of tropospheric water vapour across the tropical and sub-tropical Atlantic in March 2004 are compared to short-term forecasts of the European Centre for Medium Range Weather Forecasts (ECMWF). The humidity fields between 28° S and 36° N exhibit large inter air-mass gradients and reflect typical transport patterns of low- and mid-latitudes like convection (e.g. Hadley circulation), subsidence and baroclinic development with stratospheric intrusion. These processes re-distribute water vapour vertically such that locations with extraordinary dry/moist air-masses are observed in the lower/upper troposphere, respectively. The mixing ratios range over 3 orders of magnitude. Back-trajectories are used to trace and characterize the observed air-masses. Overall, the observed water vapour distributions are largely reproduced by the short-term forecasts at 0.25° resolution (T799/L91), the correlation ranges from 0.69 to 0.92. Locally, large differences occur due to comparably small spatial shifts in presence of strong gradients. Systematic deviations are found associated with specific atmospheric domains. The planetary boundary layer in the forecast is too moist and to shallow. Convective transport of humidity to the middle and upper troposphere tends to be overestimated. Potential impacts arising from data assimilation and model physics are considered. The matching of air-mass boundaries (transport) is discussed with repect to scales and the representativity of the 2-D sections for the 3-D humidity field. The normalized bias of the model with respect to the observations is 6%, 11% and 0% (moist model biases) for the three along-flight sections, whereby however the lowest levels are excluded.
Nitrate aerosols today and in 2030: a global simulation including aerosols and tropospheric ozone

Nitrate aerosols are expected to become more important in the future atmosphere due to the expected increase in nitrate precursor emissions and the decline of ammonium-sulphate aerosols in wide regions of this planet. The GISS climate model is used in this study, including atmospheric gas- and aerosol phase chemistry to investigate current and future (2030, following the SRES A1B emission scenario) atmospheric compositions. A set of sensitivity experiments was carried out to quantify the individual impact of emission- and physical climate change on nitrate aerosol formation. We found that future nitrate aerosol loads depend most strongly on changes that may occur in the ammonia sources. Furthermore, microphysical processes that lead to aerosol mixing play a very important role in sulphate and nitrate aerosol formation. The role of nitrate aerosols as climate change driver is analyzed and set in perspective to other aerosol and ozone forcings under pre-industrial, present day and future conditions. In the near future, year 2030, ammonium nitrate radiative forcing is about −0.14 W/m² and contributes roughly 10% of the net aerosol and ozone forcing. The present day nitrate and pre-industrial nitrate forcings are −0.11 and −0.05 W/m², respectively. The steady increase of nitrate aerosols since industrialization increases its role as a non greenhouse gas forcing agent. However, this impact is still small compared to greenhouse gas forcings, therefore the main role nitrate will play in the future atmosphere is as an air pollutant, with annual mean near surface air concentrations, in the fine particle mode, rising above 3 μg/m³ in China and therefore reaching pollution levels, like sulphate aerosols.
Efficiency of immersion mode ice nucleation on surrogates of mineral dust

A differential scanning calorimeter (DSC) was used to explore heterogeneous ice nucleation of emulsified aqueous suspensions of two Arizona test dust (ATD) samples with particle diameters of nominally 0–3 and 0–7 μm, respectively. Aqueous suspensions with ATD concentrations of 0.01–20 wt% have been investigated. The DSC thermograms exhibit a homogeneous and a heterogeneous freezing peak whose intensity ratios vary with the ATD concentration in the aqueous suspensions. Homogeneous freezing temperatures are in good agreement with recent measurements by other techniques. Depending on ATD concentration, heterogeneous ice nucleation occurred at temperatures as high as 256 K or down to the onset of homogeneous ice nucleation (237 K). For ATD-induced ice formation Classical Nucleation Theory (CNT) offers a suitable framework to parameterize nucleation rates as a function of temperature, experimentally determined ATD size, and emulsion droplet volume distributions. The latter two quantities serve to estimate the total heterogeneous surface area present in a droplet, whereas the suitability of an individual heterogeneous site to trigger nucleation is described by the compatibility function (or contact angle) in CNT. The intensity ratio of homogeneous to heterogeneous freezing peaks is in good agreement with the assumption that the ATD particles are randomly distributed amongst the emulsion droplets. The observed dependence of the heterogeneous freezing temperatures on ATD concentrations cannot be described by assuming a constant contact angle for all ATD particles, but requires the ice nucleation efficiency of ATD particles to be (log)normally distributed amongst the particles. Best quantitative agreement is reached when explicitly assuming that high-compatibility sites are rare and that therefore larger particles have on average more and better active sites than smaller ones. This analysis suggests that a particle has to have a diameter of at least 0.1 μm to exhibit on average one active site.
Perturbation of the European free troposphere aerosol by North American forest fire plumes during the ICARTT-ITOP experiment in summer 2004

During the ICARTT-ITOP Experiment in summer 2004 plumes from large wildfires in North America were transported to Central Europe at 3–8 km altitude above sea level (a.s.l.). These plumes were studied with the DLR (Deutsches Zentrum fuer Luft- und Raumfahrt) research aircraft Falcon which was equipped with an extensive set of in situ aerosol and trace gas instruments. Analyses by the Lagrangian dispersion model FLEXPART provided source regions, transport times and horizontal extent of the fire plumes. Results from the general circulation model ECHAM/MADE and data from previous aerosol studies over Central Europe provided reference vertical profiles of black carbon (BC) mass concentrations for year 2000 conditions with forest fire activities below the long-term average. Smoke plume observations yielded a BC mass fraction of total aerosol mass with respect to PM 2.5 of 2–8%. The ratio of BC mass to excess CO was 3–7.5 mg BC (g CO)−1. Even after up to 10 days of atmospheric transport, both characteristic properties were of the same order as for fresh emissions. This suggests an efficient lifting of BC from forest fires to higher altitudes with only minor scavenging removal of particulate matter. Maximum aerosol absorption coefficient values were 7–8 Mm−1 which is about two orders of magnitude above the average European free tropospheric background value. Forest fire aerosol size distributions were characterised by a strong internally mixed accumulation mode centred at modal diameters of 0.25–0.30 µm with an average distribution width of 1.30. Nucleation and small Aitken mode particles were almost completely depleted.
Ammonia at Blodgett Forest, Sierra Nevada, USA

Ammonia is a reactive trace gas that is emitted in large quantities by animal agriculture and other sources in California, which subsequently forms aerosol particulate matter, potentially affecting visibility, climate, and human health. We performed initial measurements of NH3 at the Blodgett Forest Research Station (BFRS) during a two week study in June, 2006. The site is used for ongoing air quality research and is a relatively low-background site in the foothills of the Sierra Nevada. Measured NH3 mixing ratios were quite low (<1 to ~2 ppb), contrasting with typical conditions in many parts of the Central Valley. Eddy covariance measurements showed NH3 fluxes that scaled with measured NH3 mixing ratio and calculated aerodynamic deposition velocity, suggesting dry deposition is a significant loss mechanism for atmospheric NH3 at BFRS. A simple model of NH3 transport to the site supports the hypothesis that NH3 is transported from the Valley to BFRS, but deposits on vegetation during the summer. Further work is necessary to determine whether the results obtained in this study can be generalized to other seasons.