S. W. Wood

Satellite-observed pollution from Southern Hemisphere biomass burning.

Biomass burning is a major source of pollution in the tropical Southern Hemisphere, and fine mode carbonaceous particles are produced by the same combustion processes that emit carbon monoxide (CO). In this paper we examine these emissions with data from the Terra satellite, CO profiles from the Measurement of Pollution in the Troposphere (MOPITT) instrument, and fine-mode aerosol optical depth (AOD) from the Moderate-Resolution Imaging Spectroradiometer (MODIS). The satellite measurements are used in conjunction with calculations from the MOZART chemical transport model to examine the 2003 Southern Hemisphere burning season with particular emphasis on the months of peak fire activity in September and October. Pollutant emissions follow the occurrence of dry season fires, and the temporal variation and spatial distributions of MOPITT CO and MODIS AOD are similar. We examine the outflow from Africa and South America with emphasis on the impact of these emissions on clean remote regions. We present comparisons of MOPITT observations and ground-based interferometer data from Lauder, New Zealand, which indicate that intercontinental transport of biomass burning pollution from Africa often determines the local air quality. The correlation between enhancements of AOD and CO column for distinct biomass burning plumes is very good with correlation coefficients greater than 0.8. We present a method using MOPITT and MODIS data for estimating the emission ratio of aerosol number density to CO concentration which could prove useful as input to modeling studies. We also investigate decay of plumes from African fires following export into the Indian Ocean and compare the MOPITT and MODIS measurements as a way of estimating the regional aerosol lifetime. Vertical transport of biomass burning emissions is also examined using CO profile information. Low-altitude concentrations are very high close to source regions, but further downwind of the continents, vertical mixing takes place and results in more even CO vertical distributions. In regions of significant convection, particularly in the equatorial Indian Ocean, the CO mixing ratio is greater at higher altitudes, indicating vertical transport of biomass burning emissions to the upper troposphere.

Ground‐based measurements of tropospheric and stratospheric BrO at Arrival Heights, Antarctica

Ground-based measurements of BrO slant column densities (SCDs) were performed using zenith sky DOAS (Differential Optical Absorption Spectroscopy) during autumn (February to May) and spring (August to October) of 1995 at Arrival Heights (77.8°S, 166.7°E). In both August and September, single episodes of sudden large BrO column enhancement (of magnitude 3.5 and 3.2 × 1014 molec. cm−2 respectively) were observed. The episode in August did not coincide with changes of other stratospheric parameters (OClO, NO2 and temperature). Furthermore, the diurnal variation in the SCD during these events was indicative of a tropospheric rather than a stratospheric absorber. The tropospheric BrO mixing ratios deduced from the data are similar to those observed by ground-based measurements in the Arctic boundary layer (∼30 ppt). Simultaneous balloon soundings, one during each of the two events, showed statistically significant (2 σ) tropospheric ozone depletion between 0.5 and 2 km in August and 1.5 and 2.8 km in September. Our results strongly suggest that halogen catalysed boundary layer ozone depletion not only occurs in the Arctic but also in Antarctica. This has the implication that Arctic Haze and anthropogenic influence is unlikely as a cause for this phenomenon.

Long‐term trends of inorganic chlorine from ground‐based infrared solar spectra: Past increases and evidence for stabilization

Long-term time series of hydrogen chloride (HCl) and chlorine nitrate (ClONO2) total column abundances has been retrieved from high spectral resolution ground-based solar absorption spectra recorded with infrared Fourier transform spectrometers at nine NDSC (Network for the Detection of Stratospheric Change) sites in both Northern and Southern Hemispheres. The data sets span up to 24 years and most extend until the end of 2001. The time series of Cl-y (defined here as the sum of the HCl and ClONO2 columns) from the three locations with the longest time-span records show rapid increases until the early 1990s superimposed on marked day-to-day, seasonal and inter-annual variability. Subsequently, the buildup in Cl-y slows and reaches a broad plateau after 1996, also characterized by variability. A similar time evolution is also found in the total chlorine concentration at 55 km altitude derived from Halogen Occultation Experiment (HALOE) global observations since 1991. The stabilization of inorganic chlorine observed in both the total columns and at 55 km altitude indicates that the near-global 1993 organic chlorine (CCly) peak at the Earths surface has now propagated over a broad altitude range in the upper atmosphere, though the time lag is difficult to quantify precisely from the current data sets, due to variability. We compare the three longest measured time series with two-dimensional model calculations extending from 1977 to 2010, based on a halocarbon scenario that assumes past measured trends and a realistic extrapolation into the future. The model predicts broad Cl-y maxima consistent with the long-term observations, followed by a slow Cl-y decline reaching 12-14% relative to the peak by 2010. The data reported here confirm the effectiveness of the Montreal Protocol and its Amendments and Adjustments in progressively phasing out the major man-related perturbations of the stratospheric ozone layer, in particular, the anthropogenic chlorine-bearing source gases. (Less)

Multiyear infrared solar spectroscopic measurements of HCN, CO, C2H6, and C2H2 tropospheric columns above Lauder, New Zealand (45°S latitude)

[i] Near-simultaneous, 0.0035 or 0.007 cm -1 resolution infrared solar absorption spectra of tropospheric HCN, C 2 H 2 , CO, and C 2 H 6 have been recorded from the Network for the Detection of Stratospheric Change station in Lauder, New Zealand (45.04°S, 169.68°E, 0.37 km altitude). All four molecules were measured on over 350 days with HCN and C 2 H 2 reported for the first time based on a new analysis procedure that significantly increases the effective signal-to-noise of weak tropospheric absorption features in the measured spectra. The CO measurements extend by 2.5 years a database of measurements begun in January 1994 for CO with improved sensitivity in the lower and middle troposphere. The C 2 H 6 measurements lengthen a time series begun in July 1993 with peak sensitivity in the upper troposphere. Retrievals of all four molecules were obtained with an algorithm based on the semiempirical application of the Rodgers optimal estimation technique. Columns are reported for the 0.37- to 12-km-altitude region, approximately the troposphere above the station. The seasonal cycles of all four molecules are asymmetric, with minima in March-June and sharp peaks and increased variability during August-November, which corresponds to the period of maximum biomass burning near the end of the Southern Hemisphere tropical dry season. Except for a possible HCN column decrease, no evidence was found for a statistically significant long-term trend.

Moderation of Cloud Reduction of UV in the Antarctic Due to High Surface Albedo

To gauge the impact of clouds on erythemal (sunburn causing) UV irradiances under different surface albedo conditions, UV measurements from two Antarctic sites (McMurdo and South Pole Stations) and a midlatitude site (Lauder, New Zealand) are examined. The surface albedo at South Pole remains high throughout the year, at McMurdo it has a strong annual cycle, and at Lauder it is low throughout the year. The measurements at each site are divided into clear and cloudy subsets and are compared with modeled clear-sky irradiances to assess the attenuation of UV by clouds. A radiative transfer model is also used to interpret the observations. Results show increasing attenuation of UV with increasing cloud optical depth, but a high surface albedo can moderate this attenuation as a result of multiple scattering between the surface and cloud base. This effect is of particular importance at high latitudes where snow may be present during the summer months. There is also a tendency toward greater cloud attenuation with increasing solar zenith angle.

Improvements to air mass calculations for ground-based infrared measurements

High-resolution ground-based infrared solar spectra are routinely recorded at the Network for the Detection of Stratospheric Change (NDSC) stations. These data sets play a key role in providing a long-term record of atmospheric composition and their links to climate change. The analysis of observed infrared spectra involves comparison to a computer-modeled atmosphere where knowledge of the air mass distribution is an essential component. This note summarises improvements made to an existing and widely used computer code (FSCATM) to perform refractive ray-tracing and calculation of the air mass distribution. Changes were made towards higher vertical resolution in the troposphere and increased numerical precision. The revised FSCATM improves the analysis of infrared spectra mostly through the more accurate representation of the temperature profile. Air mass differences with respect to earlier versions are documented and are typically <0.7%, exceptions being extreme cases of inversion layers. The current version provides ray tracing and air mass calculations for any terrestrial observation site. The output files are reported in a format compatible with the SFIT and SFIT2 retrieval algorithms, which are widely used for NDSC infrared atmospheric studies. The improved computer code, documentation, reference profiles, and test cases are available electronically.

Correlation relationships of stratospheric molecular constituents from high spectral resolution, ground‐based infrared solar absorption spectra

Comparisons of chemically active species with chemically inert tracers are useful to quantify transport and mixing and assess the accuracy of model predictions. We report measurements of chemically active species and chemically inert tracers in the stratosphere derived from the analysis of infrared solar absorption spectra recorded with a ground-based Fourier transform spectrometer operated typically at 0.005- to 0.01-cm−1 spectral resolution. The measurements were recorded from Kitt Peak in southern Arizona (latitude 31.9°N, 111.6°W, 2.09 km altitude). Time series of N2O, CH4, O3, and HNO3 vertical profiles have been retrieved from measurements in microwindows. From these results, correlations between N2O and CH4 stratospheric mixing ratios and between O3 and HNO3 lower stratospheric mixing ratios have been derived. The measured correlations between N2O versus CH4 mixing ratios are compact and show little variability with respect to season in quantitative agreement with Atmospheric Trace Molecule Spectroscopy Experiment (ATMOS) spring and autumn measurements recorded near the same latitude. Lower stratospheric O3 versus HNO3 mixing ratios measured during low to moderate aerosol loading time periods also show a compact relations though the HNO3/O3 slope is a factor of 2 lower than obtained from November 1994 ATMOS measurements near the same latitude. We also compare Kitt Peak and ATMOS N2O versus CH4 and O3 versus HNO3 relations obtained by averaging the measurements over two broad stratospheric layers. This comparison avoids bias from the a priori profiles and the limited vertical resolution of the ground-based observations.

Intercomparison of total ozone data from a Dobson spectrophotometer, TOMS, visible wavelength spectrometer, and ozonesondes

Comparisons of total column ozone measurements from three ground-based instruments (Dobson spectrophotometer, ozonesonde, and visible wavelength grating spectrometer) and the TOMS instrument are presented for the period 1991 to 1994 at Arrival Heights/McMurdo, Antarctica. The primary purpose of these comparisons is to investigate the accuracy of the visible spectrometer, while a second aim is to compare version 6 and version 7 TOMS satellite retrievals with the ground-based measurements. While the Dobson, TOMS and ozonesonde measurements show good agreement, there is a seasonal dependence between data from the visible wavelength spectrometer and each of the other three instruments. However, the visible spectrometer produces valuable data for the late autumn and early spring, when data are not available from the Dobson and TOMS.

Sustainability and greenhouse gases: What are the issues for New Zealand?

Abstract One of the real challenges for the scientific community in the next decade will be in the production and validation of atmospheric composition data, not to the normally accepted scientific criterion and standards but to and within a new legalistic framework. As the issues created by the implementation and application of the Kyoto Protocol come into force, the attribution of sources of greenhouse gases will become critical, as will indeed the proof of compliance with Kyoto Protocol conditions. This paper discusses some of the drivers of global change to set in context the changes that are occurring in the atmosphere and shows that although the term sustainability is often used implying some semi-equilibrium state, the atmosphere is unlikely to be in a quasi-equilibrium state over the next 200 years. Examples of the special problems faced by New Zealand are used to illustrate the complexity of this issue.

A community diagnostic tool for chemistry climate model validation

This technical note presents an overview of the Chemistry-Climate Model Validation Diagnostic (CCMValDiag) tool for model evaluation. The CCMVal-Diag tool is a flexible and extensible open source package that facilitates the complex evaluation of global models. Models can be compared to other models, ensemble members (simulations with the same model), and/or many types of observations. The initial construction and application is to coupled chemistry-climate models (CCMs) participating in CCMVal, but the evaluation of climate models that submitted output to the Coupled Model Intercomparison Project (CMIP) is also possible. The package has been used to assist with analysis of simulations for the 2010 WMO/UNEP Scientific Ozone Assessment and the SPARC Report on the Evaluation of CCMs. The CCMVal-Diag tool is described and examples of how it functions are presented, along with links to detailed descriptions, instructions and source code. The CCMVal-Diag tool supports model development as well as quantifies model changes, both for different versions of individual models and for different generations of community-wide collections of models used in international assessments. The code allows further extensions by different users for different applications and types, e.g. to other components of the Earth system. User modifications are encouraged and easy to perform with minimum coding.