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Optical properties of humic-like substances (HULIS) in biomass-burning aerosols

We present here the optical properties of humic-like substances (HULIS) isolated from the fine fraction of biomass-burning aerosol collected in the Amazon basin during the LBA-SMOCC (Large scale Biosphere atmosphere experiment in Amazonia – SMOke aerosols, Clouds, rainfall and Climate) experiment in September 2002. From the isolated HULIS, aerosol particles were generated and their scattering and absorption coefficients measured. The size distribution and mass of the particles were also recorded. The value of the index of refraction was derived from "closure" calculations based on particle size, scattering and absorption measurements. On average, the complex index of refraction at 532 nm of HULIS collected during day and nighttime was 1.65–0.0019i and 1.69–0.0016i, respectively. In addition, the imaginary part of the complex index of refraction was calculated using the measured absorption coefficient of the bulk HULIS. The mass absorption coefficient of the HULIS at 532 nm was found to be quite low (0.031 and 0.029 m2 g−1 for the day and night samples, respectively). However, due to the high absorption Ångström exponent (6–7) of HULIS, the specific absorption increases substantially towards shorter wavelengths (~2–3 m2 g−1 at 300 nm), causing a relatively high (up to 50%) contribution to the light absorption of our Amazonian aerosol at 300 nm. For the relative contribution of HULIS to light absorption in the entire solar spectrum, lower values (6.4–8.6%) are obtained, but those are still not negligible.
Technical note: Recursive rediscretisation of geo-scientific data in the Modular Earth Submodel System (MESSy)

This technical note describes a method for the rediscretisation of "gridded" geo-scientific data. A recursive algorithm (NREGRID) is derived to solve the rediscretisation problem for orthogonal grids (including curvilinear) of arbitrary dimension. The algorithm is used within the program NCREGRID to handle geo-scientific data. These data are typically 2-dimensional (latitude-longitude grid), or 3-dimensional (latitude-longitude grid with a vertical pressure, or hybrid pressure coordinate, as used in atmospheric modelling). NCREGRID can be used as stand-alone program for the transformation ("regridding") of data from and to data files in netCDF format. Moreover, NCREGRID constitutes the core of the Modular Earth Submodel System (MESSy) data import interface, providing a powerful tool for accessing data independently of the applied grid resolution ("automatic regridding").
Measuring atmospheric CO2 from space using Full Spectral Initiation (FSI) WFM-DOAS

Satellite measurements of atmospheric CO2 concentrations are a rapidly evolving area of scientific research which can help reduce the uncertainties in the global carbon cycle fluxes and provide insight into surface sources and sinks. One of the emerging CO2 measurement techniques is a relatively new retrieval algorithm called Weighting Function Modified Differential Optical Absorption Spectroscopy (WFM-DOAS) that has been developed by Buchwitz et al. (2000). This algorithm is designed to measure the total columns of CO2 (and other greenhouse gases) through the application to spectral measurements in the near infrared (NIR), made by the SCIAMACHY instrument on-board ENVISAT. The algorithm itself is based on fitting the logarithm of a model reference spectrum and its derivatives to the logarithm of the ratio of a measured nadir radiance and solar irradiance spectrum. In this work, a detailed error assessment of this technique has been conducted and it has been found necessary to include suitable a priori information within the retrieval in order to minimize the errors on the retrieved CO2 columns. Hence, a more flexible implementation of the retrieval technique, called Full Spectral Initiation (FSI) WFM-DOAS, has been developed which generates a reference spectrum for each individual SCIAMACHY observation using the estimated properties of the atmosphere and surface at the time of the measurement. Initial retrievals over Siberia during the summer of 2003 show that the measured CO2 columns are not biased from the input a priori data and that whilst the monthly averaged CO2 distributions contain a high degree of variability, they also contain interesting spatial features.
Importance of the surface reaction OH + Cl− on sea salt aerosol for the chemistry of the marine boundary layer – a model study

The reaction of the hydroxyl radical with chloride on the surface of sea salt aerosol producing gas phase Cl2 and particulate OH− and its implications for the chemistry of the marine boundary layer under coastal, remote, and very remote conditions have been investigated with a numerical model. This reaction had been suggested by Laskin et al. (2003) to play a major role in the sulfur cycle in the marine boundary layer by increasing the sulfate production in sea salt by O3 oxidation due to the additional production of alkalinity in the particle. Based on literature data a new "best estimate" for the rate coefficient of the reaction was deduced and applied, showing that the additional initial sulfate production by this reaction is less than 1%, therefore having only a minor impact on sulfate production. Even though the gas phase concentration of Cl2 increased strongly in the model, the concentration of Cl radicals increased by less than 5% for the "best guess" case. Additional feedbacks between the cycles of chlorine and sulfur in the marine boundary layer are discussed as well as a two-stage acidification of large fresh sea salt aerosol.
Combined observational and modeling based study of the aerosol indirect effect

The indirect effect of aerosols via liquid clouds is investigated by comparing aerosol and cloud characteristics from the Global Climate Model CAM-Oslo to those observed by the MODIS instrument onboard the TERRA and AQUA satellites http://modis.gsfc.nasa.gov). The comparison is carried out for 15 selected regions ranging from remote and clean to densely populated and polluted. For each region, the regression coefficient and correlation coefficient for the following parameters are calculated: Aerosol Optical Depth vs. Liquid Cloud Optical Thickness, Aerosol Optical Depth vs. Liquid Cloud Droplet Effective Radius and Aerosol Optical Depth vs. Cloud Liquid Water Path. Modeled and observed correlation coefficients and regression coefficients are then compared for a 3-year period starting in January 2001. Additionally, global maps for a number of aerosol and cloud parameters crucial for the understanding of the aerosol indirect effect are compared for the same period of time. Significant differences are found between MODIS and CAM-Oslo both in the regional and global comparison. However, both the model and the observations show a positive correlation between Aerosol Optical Depth and Cloud Optical Depth in practically all regions and for all seasons, in agreement with the current understanding of aerosol-cloud interactions. The correlation between Aerosol Optical Depth and Liquid Cloud Droplet Effective Radius is variable both in the model and the observations. However, the model reports the expected negative correlation more often than the MODIS data. Aerosol Optical Depth is overall positively correlated to Cloud Liquid Water Path both in the model and the observations, with a few regional exceptions.
Technical note: Implementation of prescribed (OFFLEM), calculated (ONLEM), and pseudo-emissions (TNUDGE) of chemical species in the Modular Earth Submodel System (MESSy)

We present the submodels OFFLEM, ONLEM, and TNUDGE for the Modular Earth Submodel System (MESSy). Prescribed emissions from input files are handled by OFFLEM. ONLEM deals with online-calculated emissions, i.e., emissions that are calculated during the simulation. The submodel TNUDGE uses the "tracer nudging" technique for pseudo-sources and -sinks. For species with highly uncertain emission fluxes and/or with sufficiently long lifetimes, e.g., CH4, it is common to create such pseudo-fluxes by prescribing the observed mixing ratio of the species at a given boundary (e.g., the mixing ratio of methane at the surface, or the ozone mixing ratio at the tropopause). All three submodels substantially simplify the inclusion of emissions into a model. Specific emissions can easily be switched on or off. New prescribed emissions can be included without rewriting any code. New online emissions only require one additional subroutine containing the new parameterization. A major advantage is that input fields at arbitrary resolution can be used. The problem of incompatible grids between emission data and model is overcome by utilizing the MESSy data import interface. To further simplify the creation of new offline emission data, the preprocessing program EDGAR2NC is provided. EDGAR2NC transforms files from the EDGAR format into the netCDF format which is required by OFFLEM. The presented routines are a part of the community modeling project MESSy and can be made available for use to the atmospheric modeling community.
The effects of convection on the summertime mid-latitude overworld

Halogen Occultation Experiment measurements of H2O are used to investigate the influence of mid-latitude convection on the summertime overworld between 30° N and 40° N. We find that most of the convective influence over this latitude range occurs over the Asian monsoon and over North America. Over North America, the effects of convection extend to ~410 K (17.5 km). Over Asia, the effects of convection extend to ~460 K (19 km), about 50 K (1.5 km) higher than over North America.
Liquid particle composition and heterogeneous reactions in a mountain wave Polar Stratospheric Cloud

Mountain wave polar stratospheric clouds (PSCs) were detected on 8 February 2003 above the Scandinavian Mountains by in-situ instruments onboard the M55 Geophysica aircraft. PSC particle composition, backscatter and chlorine activation for this case are studied with a recently developed non-equilibrium microphysical box model for liquid aerosol. Results from the microphysical model, run on quasi-lagrangian trajectories, show that the PSC observed was composed of supercooled ternary (H2O/HNO3/H2SO4) solution (STS) particles, which are out of equilibrium with the gas phase. The measured condensed nitric acid and aerosol backscatter of the PSC can well be simulated with the model. Up to 0.15 ppbv Cl2 can be released by the PSC within 2 h, showing the propensity of these small-scale clouds for chlorine activation. Equilibrium calculations – of the sort commonly used in large scale chemistry transport models – overestimate the measured condensed nitrate by up to a factor of 3, and overestimates chlorine activation by 10%, in this mountain wave cloud.
Evaluated kinetic and photochemical data for atmospheric chemistry: Volume II – gas phase reactions of organic species

This article, the second in the series, presents kinetic and photochemical data evaluated by the IUPAC Subcommittee on Gas Kinetic Data Evaluation for Atmospheric Chemistry. It covers the gas phase and photochemical reactions of Organic species, which were last published in 1999, and were updated on the IUPAC website in late 2002, and subsequently during the preparation of this article. The article consists of a summary table of the recommended rate coefficients, containing the recommended kinetic parameters for the evaluated reactions, and eight appendices containing the data sheets, which provide information upon which the recommendations are made.
Search for evidence of trend slow-down in the long-term TOMS/SBUV total ozone data record: the importance of instrument drift uncertainty

We have developed a merged ozone data set (MOD) for the period October 1978 through June 2006 combining total ozone measurements (Version 8 retrieval) from the TOMS (Nimbus 7, Earth Probe) and SBUV/SBUV2 (Nimbus 7, NOAA 9/11/16) series of satellite instruments. We use the MOD data set to search for evidence of ozone recovery in response to the observed leveling off of chlorine and bromine compounds in the stratosphere. A crucial step in any time series analysis is the evaluation of uncertainties. In addition to the standard statistical time series uncertainties, we evaluate the possible instrument drift uncertainty for the MOD data set. We combine these two sources of uncertainty and apply them to a cumulative sum of residuals (CUSUM) analysis for trend slow-down. For the extra-polar mean between 60° S and 60° N, the apparent slow-down in trend is found to be clearly significant if instrument uncertainties are ignored. When instrument uncertainties are added, the slow-down becomes marginally significant at the 2σ level. For the mid-latitudes of the northern hemisphere (30° to 60° N) the trend slow-down is highly significant at the 2σ level, while in the southern hemisphere the trend slow-down has yet to meet the 2σ significance criterion. The rate of change of chlorine/bromine compounds is similar in both hemispheres, and we expect the ozone response to be similar in both hemispheres as well. The asymmetry in the trend slow-down between hemispheres likely reflects the influence of dynamical variability, and thus a clearly statistically significant response of total ozone to the leveling off of chlorine and bromine in the stratosphere is not yet indicated.