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Evaluation of near-tropopause ozone distributions in the Global Modeling Initiative combined stratosphere/troposphere model with ozonesonde data

The NASA Global Modeling Initiative has developed a combined stratosphere/troposphere chemistry and transport model which fully represents the processes governing atmospheric composition near the tropopause. We evaluate model ozone distributions near the tropopause, using two high vertical resolution monthly mean ozone profile climatologies constructed with ozonesonde data, one by averaging on pressure levels and the other relative to the thermal tropopause. At the tropopause, model ozone is high-biased in the SH tropics and NH midlatitudes by ~45% in a 4° latitude ×5° longitude model simulation. Doubling the resolution to 2°×2.5° increases the NH high bias to ~60%, and reduces the tropical bias to ~30%, apparently due to decreased horizontal transport between the tropics and extratropics in the higher-resolution simulation. These ozone biases do not appear to be due to an overly vigorous residual circulation, insufficient convection, or excessive stratosphere/troposphere exchange, and so may be due to insufficient vertical resolution or excessive vertical diffusion near the tropopause. In the upper troposphere and lower stratosphere, model/measurement intercomparisons are strongly affected by the averaging technique. Compared to the pressure-averaged climatology, NH and tropical mean model lower stratospheric biases are >20%. In the upper troposphere, the 2°×2.5° simulation shows mean high biases of ~20% and ~35% during April in the tropics and NH midlatitudes, respectively. This apparently good model/measurement agreement degrades when relative-to-tropopause averages are considered, with upper troposphere high biases of ~30% and 70% in the tropics and NH midlatitudes. This occurs because relative-to-tropopause averaging better preserves the larger cross-tropopause O3 gradients which are seen in the daily sonde data, but not in daily model profiles. Relative-to-tropopause averages therefore more accurately reveal model/measurement discrepancies. The relative annual cycle of ozone near the tropopause is reproduced very well in the model Northern Hemisphere midlatitudes. In the tropics, the model amplitude of the near-tropopause annual cycle is weak. This is likely due to the annual amplitude of mean vertical upwelling near the tropopause, which analysis suggests is ~30% weaker than in the real atmosphere.
Discriminating raining from non-raining clouds at mid-latitudes using meteosat second generation daytime data

A new method for the delineation of precipitation during daytime using multispectral satellite data is proposed. The approach is not only applicable to the detection of mainly convective precipitation by means of the commonly used relation between infrared cloud top temperature and rainfall probability but enables also the detection of stratiform precipitation (e.g. in connection with mid-latitude frontal systems). The presented scheme is based on the conceptual model that precipitating clouds are characterized by a combination of particles large enough to fall, an adequate vertical extension (both represented by the cloud water path; cwp), and the existence of ice particles in the upper part of the cloud. The technique considers the VIS0.6 and the NIR1.6 channel to gain information about the cloud water path. Additionally, the brightness temperature differences ΔT8.7-10.8 and ΔT10.8-12.1 are considered to supply information about the cloud phase. Rain area delineation is realized by using a minimum threshold of the rainfall confidence. To obtain a statistical transfer function between the rainfall confidence and the four parameters VIS<sub0.6, NIR1.6, Δ T8.7-10.8 and Δ T10.8-12.1, the value combinations of these four variables are compared to ground based radar data. The retrieval is validated against independent radar data not used for deriving the transfer function and shows an encouraging performance as well as clear improvements compared to existing optical retrieval techniques using only IR thresholds for cloud top temperature.
The potential importance of frost flowers, recycling on snow, and open leads for ozone depletion events

We present model studies with the one-dimensional model MISTRA to investigate the potential role of frost flowers, recycling on snow, and open leads in the depletion of tropospheric ozone in the Arctic spring. In our model, we assumed frost flower aerosols to be the major source of bromine. We show that a major ozone depletion event can be satisfactorily reproduced only if the recycling on snow of deposited bromine into gas phase bromine is assumed. In the model, this cycling is more efficient than the bromine explosion process and maintains sufficiently high levels of bromine to deplete ozone down to few nmol mol−1 within four days. We assessed the influence of different surface combinations (open lead/frost flowers) on the chemistry in the model. Results showed noticeable modifications affecting the composition of aerosols and the deposition velocities. A model run with a series of coupled frost flower fields and open leads, separated by large areas of snow, showed results comparable with field observations. In addition, we studied the effects of modified temperature of either the frost flower field or the ambient airmass. A warmer frost flower field increases the relative humidity and the aerosol deposition rate. The deposition/re-emission process gains in importance, inducing more reactive bromine in the gas phase, and a stronger ozone depletion. A decrease of 1K in airmass temperature shows in our model that the aerosol uptake capacities of all gas phase species substantially increases, leading to enhanced uptake of acids from the gas phase. Consequently, the so-called bromine explosion accelerated and O3 mixing ratios decreased. In our model representation, variations in wind speed affected the aerosol source function and influenced the amount of bromine in the atmosphere and thus the ozone depletion strength. Recent studies have suggested the important role of the precipitation of calcium carbonate (CaCO3) out of the brine layer for the possible acidification of the liquid phase by acid uptake. Our investigation showed that this precipitation is a crucial process for the timing of the bromine explosion in aerosols. Nevertheless, model runs with either 50% precipitation or complete precipitation displayed a relatively weak difference in ozone mixing ratios after four simulated days. By considering conditions typical for "Arctic Haze" pollution events at the start of the run we obtained a low pH in frost flower aerosols due to a greater mixing ratio of SO2, and a strong recycling efficiency via large aerosol number concentration. The aerosol acidification during a haze event most likely intensifies the ozone depletion strength and occurrence. The comparison between our modeled deposition on snow and sampled snow at Barrow (Alaska) shows that approximately 75% of deposited bromine may be re-emitted into the gas phase as Br2/BrCl. Among several non-halogen fluxes from the snow, model simulations showed that only HONO affects the chemistry. Finally, we investigated the release of Br2 potentially produced by heterogeneous reactions directly on frost flowers. In this case, we obtained unrealistic results of aerosol compositions and deposition rates on snow compared to observations in the Arctic.
Validation of ACE-FTS v2.2 methane profiles from the upper troposphere to the lower mesosphere

The ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) solar occultation instrument that was launched onboard the Canadian SCISAT-1 satellite in August 2003 is measuring vertical profiles from the upper troposphere to the lower mesosphere for a large number of atmospheric constituents. Methane is one of the key species. The version v2.2 data of the ACE-FTS CH4 data have been compared to correlative satellite, balloon-borne and ground-based Fourier transform infrared remote sensing data to assess their quality. The comparison results indicate that the accuracy of the data is within 10% in the upper troposphere – lower stratosphere, and within 25% in the middle and higher stratosphere up to the lower mesosphere (<60 km). The observed differences are generally consistent with reported systematic uncertainties. ACE-FTS is also shown to reproduce the variability of methane in the stratosphere and lower mesosphere.
Global modeling of secondary organic aerosol formation from aromatic hydrocarbons: high- vs. low-yield pathways

Formation of SOA from the aromatic species toluene, xylene, and, for the first time, benzene, is added to a global chemical transport model. A simple mechanism is presented that accounts for competition between low and high-yield pathways of SOA formation, wherein secondary gas-phase products react further with either nitric oxide (NO) or hydroperoxy radical (HO2) to yield semi- or non-volatile products, respectively. Aromatic species yield more SOA when they react with OH in regions where the [NO]/[HO2] ratios are lower. The SOA yield thus depends upon the distribution of aromatic emissions, with biomass burning emissions being in areas with lower [NO]/[HO2] ratios, and the reactivity of the aromatic with respect to OH, as a lower initial reactivity allows transport away from industrial source regions, where [NO]/[HO2] ratios are higher, to more remote regions, where this ratio is lower and, hence, the ultimate yield of SOA is higher. As a result, benzene is estimated to be the most important aromatic species with regards to global formation of SOA, with a total production nearly equal that of toluene and xylene combined. Global production of SOA from aromatic sources via the mechanisms identified here is estimated at 3.5 Tg/yr, resulting in a global burden of 0.08 Tg, twice as large as previous estimates. The contribution of these largely anthropogenic sources to global SOA is still small relative to biogenic sources, which are estimated to comprise 90% of the global SOA burden, about half of which comes from isoprene. Uncertainty in these estimates owing to factors ranging from the atmospheric relevance of chamber conditions to model deficiencies result in an estimated range of SOA production from aromatics of 2–12 Tg/yr. Though this uncertainty range affords a significant anthropogenic contribution to global SOA, it is evident from comparisons to recent observations that additional pathways for production of anthropogenic SOA still exist beyond those accounted for here. Nevertheless, owing to differences in spatial distributions of sources and seasons of peak production, regions exist in which aromatic SOA produced via the mechanisms identified here are predicted to contribute substantially to, and even dominate, the local SOA concentrations, such as outflow regions from North America and South East Asia during the wintertime, though total modeled SOA concentrations there are small (~0.1 μg/m3).
SALSA – a Sectional Aerosol module for Large Scale Applications

The sectional aerosol module SALSA is introduced. The model has been designed to be implemented in large scale climate models, which require both accuracy and computational efficiency. We have used multiple methods to reduce the computational burden of different aerosol processes to optimize the model performance without losing physical features relevant to problematics of climate importance. The optimizations include limiting the chemical compounds and physical processes available in different size sections of aerosol particles; division of the size distribution into size sections using size sections of variable width depending on the sensitivity of microphysical processing to the particles sizes; the total amount of size sections to describe the size distribution is kept to the minimum; furthermore, only the relevant microphysical processes affecting each size section are calculated. The ability of the module to describe different microphysical processes was evaluated against explicit microphysical models and several microphysical models used in air quality models. The results from the current module show good consistency when compared to more explicit models. Also, the module was used to simulate a new particle formation event typical in highly polluted conditions with comparable results to more explicit model setup.
Local anthropogenic impact on particulate elemental carbon concentrations at Summit, Greenland

Summit, Greenland is a remote Arctic research station allowing for field measurements at the highest point of the Greenland Ice Sheet. Due to the current reliance on diesel generators for electricity at Summit, unavoidable local emissions are a potential contamination threat to the measurement of combustion-related species in the air and snow. The effect of fossil-fuel combustion on particulate elemental carbon (EC) is assessed by a combination of ambient measurements (~1 km from the main camp), a series of snow pits, and Gaussian plume modeling. Ambient measurements indicate that the air directly downwind of the research station generators experiences particulate absorption coefficient (closely related to EC) values that are up to a factor of 200 higher than the summer 2006 non-camp-impacted ambient average. Local anthropogenic influence on snow EC content is also evident. The average EC concentration in 1-m snow pits in the "clean air" sector of Summit Camp are a factor of 1.8–2.4 higher than in snow pits located 10 km and 20 km to the north ("downwind") and south ("upwind") of the research site. Gaussian plume modeling performed using meteorological data from years 2003–2006 suggests a strong angular dependence of anthropogenic impact, with highest risk to the northwest of Summit Camp and lowest to the southeast. Along a transect to the southeast (5 degree angle bin), the modeled frequency of significant camp contribution to atmospheric EC (i.e. camp-produced EC>summer 2006 average EC) at a distance of 0.5 km, 10 km, and 20 km is 1%, 0.2%, and 0.05%, respectively. According to both the snow pit and model results, a distance exceeding 10 km towards the southeast is expected to minimize risk of contamination. These results also suggest that other remote Arctic monitoring stations powered by local fuel combustion may need to account for local air and snow contamination in field sampling design and data interpretation.
A model intercomparison analysing the link between column ozone and geopotential height anomalies in January

A statistical framework to evaluate the performance of chemistry-climate models with respect to the interaction between meteorology and column ozone during northern hemisphere mid-winter, in particularly January, is used. Different statistical diagnostics from four chemistry-climate models (E39C, ME4C, UMUCAM, ULAQ) are compared with the ERA-40 re-analysis. First, we analyse vertical coherence in geopotential height anomalies as described by linear correlations between two different pressure levels (30 and 200 hPa) of the atmosphere. In addition, linear correlations between column ozone and geopotential height anomalies at 200 hPa are discussed to motivate a simple picture of the meteorological impacts on column ozone on interannual timescales. Secondly, we discuss characteristic spatial structures in geopotential height and column ozone anomalies as given by their first two empirical orthogonal functions. Finally, we describe the covariance patterns between reconstructed anomalies of geopotential height and column ozone. In general we find good agreement between the models with higher horizontal resolution (E39C, ME4C, UMUCAM) and ERA-40. The Pacific-North American (PNA) pattern emerges as a useful qualitative benchmark for the model performance. Models with higher horizontal resolution and high upper boundary (ME4C and UMUCAM) show good agreement with the PNA tripole derived from ERA-40 data, including the column ozone modulation over the Pacfic sector. The model with lowest horizontal resolution does not show a classic PNA pattern (ULAQ), and the model with the lowest upper boundary (E39C) does not capture the PNA related column ozone variations over the Pacific sector. Those discrepancies have to be taken into account when providing confidence intervals for climate change integrations.
Ozone profile retrieval from limb scatter measurements in the HARTLEY bands: further retrieval details and profile comparisons

SCIAMACHY limb scatter radiance measurements at selected wavelengths in the HARTLEY bands have been used to retrieve ozone profiles in the upper stratosphere and lower mesosphere. Comparisons with profiles measured by a ground based radiometer in Norway, MIPAS on board ENVISAT, HALOE on UARS and MLS on AURA indicate an agreement within 15% between 40 and 55 km and show that the retrieval provides reliable ozone profiles at these altitudes. Above 55 km, an increasing overestimation is observed. Beside the profile comparisons, further retrieval features of the current retrieval (version 1.26) are described.
Ion-mediated nucleation as an important global source of tropospheric aerosols

Aerosol nucleation events have been observed at a variety of locations worldwide, and may have significant climatic and health implications. While ions have long been suggested as favorable nucleation embryos, their significance as a global source of particles has remained uncertain. Here, an ion-mediated nucleation (IMN) mechanism, which incorporates new thermodynamic data and physical algorithms, has been integrated into a global chemical transport model (GEOS-Chem) to study ion-mediated particle formation in the global troposphere. The simulated annual mean results have been compared to a comprehensive set of data relevant to particle nucleation around the globe. We show that predicted annual spatial patterns of particle formation agree reasonably well with land-, ship-, and aircraft-based observations. Our simulations show that, globally, IMN in the boundary layer is largely confined to two broad latitude belts: one in the northern hemisphere (~20° N–70° N), and one in the southern hemisphere (~30° S–90° S). In the middle latitude boundary layer over continents, the annual mean IMN rates are generally above 104 cm−3day−1, with some hot spots reaching 105 cm−3day−1. The zonally-averaged vertical distribution of IMN rates indicates that IMN is significant in the tropical upper troposphere, the entire middle latitude troposphere, and over Antarctica. Comparing the relative strengths of particle sources due to IMN and due to primary particle emissions demonstrates that IMN is significant on a global scale. Further research is needed to reduce modeling uncertainties and to understand the ultimate contribution of freshly nucleated particles to the abundance of cloud condensation nuclei.