A. T. J. de Laat

Evidence for long-range transport of Carbon Monoxide in the Southern Hemisphere from SCIAMACHY observations

This paper gives an overview of the results published by [1],[2], and [3]. The precision of the SCIAMACHY carbon monoxide (CO) total columns depends on the random instrument-noise error and is generally within 10% for monthly means. SCIAMACHY CO total columns agree well with chemistry-transport model simulations using the GFEDv2 biomass-burning emission data base. Enhanced CO columns are seen with SCIAMACHY over Australia during its biomass-burning season in local Spring. It is shown that the enhancements over Australian biomass-burning areas contain a large contribution of CO from South American biomass-burning regions. The results indicate that SCIAMACHY can be used to study both longe-range transport and emission sources of CO.

Tropospheric O3 distribution over the Indian Ocean during spring 1995 evaluated with a chemistry-climate model

An analysis of tropospheric O3 over the Indian Ocean during spring 1995 is presented based on O3 soundings and results from the European Centre Hamburg (ECHAM) chemistry-general circulation model. The ECHAM model is nudged toward actual meteorology using European Centre for Medium-Range Weather Forecasts analyses, to enable a direct comparison between model results and in situ observations. The model reproduces observed CO levels in different air mass categories. The model also reproduces the general tendencies and the diurnal variation in the observed surface pressure, although the amplitude of the diurnal variation in the amplitude is underestimated. The model simulates the general O3 tendencies as seen in the sonde observations. Tropospheric O3 profiles were characterized by low surface concentrations (<10 ppbv), midtropospheric maxima (60–100 ppbv, at 700–250 hPa) and upper tropospheric minima (<20 ppbv, at 250–100 hPa). Large-scale upper tropospheric O3 minima were caused by connective transport of O3-depleted boundary layer air in the intertropical convergence zone (ITCZ). Similarly, an upper tropospheric O3 minimum was caused by Cyclone Marlene south of the ITCZ. The midtropospheric O3 maxima were caused by transport of polluted African air. The ECHAM model appears to overestimate surface O3 levels and does not reproduce the diurnal variations very well. This could be related to unaccounted multiphase O3 destruction mechanisms involving low level clouds and aerosols, and missing halogen chemistry.

Model analysis of trace gas measurements and pollution impact during INDOEX

An analysis of acetone (CH3COCH3) and acetonitrile (CH3CN) measurements, performed during the Indian Ocean Experiment (INDOEX), using a chemistry general circulation model is presented. A comparison with measurements indicates that the model simulates realistic CO and acetone distributions, except towards the Indian west coast near the surface. The latter may be related to a sea breeze circulation at the Indian west coast, which is not resolved by the model. A comparison of the measured and modeled correlation between CO and acetone indicates the presence of a background marine acetone source. A model sensitivity study suggests a global marine emission strength of 15-20 Tg acetone year -1 , which is a significant contribution to the estimated global acetone source of 56 (37-80) Tg acetone year -1 . The comparison of measured and modeled CO-acetonitrile correlation from surface measurements indicates that a model sink of acetonitrile in the marine boundary layer is missing. A model sensitivity study suggests that this could be dry deposition (deposition velocity estimate: 0.01-0.05 cm s -1 ) on the ocean surface. A comparison of measured and modeled tropospheric acetonitrile indicates that the model overestimates the free tropospheric acetonitrile mixing ratios up to a factor of three, which points to a missing free tropospheric sink of acetonitrile in the model. A possible explanation may be stratospheric loss and subsequent stratosphere-troposphere exchange, which was not included in the model.

Quantitative analysis of SCIAMACHY carbon monoxide total column measurements

Global tropospheric ozone distributions, budgets, and radiative forcings from an ensemble of 26 state-of-the-art atmospheric chemistry models have been intercompared and synthesized as part of a wider study into both the air quality and climate roles of ozone. Results from three 2030 emissions scenarios, broadly representing “optimistic,” “likely,” and “pessimistic” options, are compared to a base year 2000 simulation. This base case realistically represents the current global distribution of tropospheric ozone. A further set of simulations considers the influence of climate change over the same time period by forcing the central emissions scenario with a surface warming of around 0.7K. The use of a large multimodel ensemble allows us to identify key areas of uncertainty and improves the robustness of the results. Ensemble mean changes in tropospheric ozone burden between 2000 and 2030 for the 3 scenarios range from a 5% decrease, through a 6% increase, to a 15% increase. The intermodel uncertainty (±1 standard deviation) associated with these values is about ±25%. Model outliers have no significant influence on the ensemble mean results. Combining ozone and methane changes, the three scenarios produce radiative forcings of -50, 180, and 300 mW m-2, compared to a CO2 forcing over the same time period of 800–1100 mW m-2. These values indicate the importance of air pollution emissions in short- to medium-term climate forcing and the potential for stringent/lax control measures to improve/worsen future climate forcing. The model sensitivity of ozone to imposed climate change varies between models but modulates zonal mean mixing ratios by ±5 ppbv via a variety of feedback mechanisms, in particular those involving water vapor and stratosphere-troposphere exchange. This level of climate change also reduces the methane lifetime by around 4%. The ensemble mean year 2000 tropospheric ozone budget indicates chemical production, chemical destruction, dry deposition and stratospheric input fluxes of 5100, 4650, 1000, and 550 Tg(O3) yr-1, respectively. These values are significantly different to the mean budget documented by the Intergovernmental Panel on Climate Change (IPCC) Third Assessment Report (TAR). The mean ozone burden (340 Tg(O3)) is 10% larger than the IPCC TAR estimate, while the mean ozone lifetime (22 days) is 10% shorter. Results from individual models show a correlation between ozone burden and lifetime, and each models ozone burden and lifetime respond in similar ways across the emissions scenarios. The response to climate change is much less consistent. Models show more variability in the tropics compared to midlatitudes. Some of the most uncertain areas of the models include treatments of deep tropical convection, including lightning NO x production; isoprene emissions from vegetation and isoprenes degradation chemistry; stratosphere-troposphere exchange; biomass burning; and water vapor concentrations.

Source analysis of carbon monoxide pollution during INDOEX 1999

A source analysis of carbon monoxide (CO) over the Indian Ocean is presented using marked tracers in a chemistry general circulation model. The model includes a nonmethane hydrocarbon chemistry scheme and has been used at two different resolutions (3.75° × 3.75° and 1.9° × 1.9°). European Centre for Medium-Range Weather Forecasts meteorological analyses have been assimilated into the model to represent actual meteorology during February and March of 1999. A comparison with measurements indicates that the model simulates realistic CO distributions. In general, the model performance is more realistic at higher resolution. Discrepancies exist close to the Indian coasts, possibly related to a sea breeze circulation at the Indian west coast, not resolved by the model. Discrepancies are also found in the vicinity of convection at the Intertropical Convergence Zone (ITCZ). The marked tracer study suggests that biofuel use and agricultural waste burning in India are major CO sources for the Indian Ocean north of the ITCZ, with minor contributions from Middle East, China, and Southeast Asia. In the much cleaner boundary layer over the southern Indian Ocean, CO from hydrocarbon oxidation is a dominant source. There are no other regions around the globe where biofuel use and biomass burning contribute so much to the CO mixing ratios. In general, most of the Asian CO over the Indian Ocean remains north of the ITCZ, although some of the CO is transported to the southern hemisphere in the free troposphere near the African east coast.

Comparing optimized CO emission estimates using MOPITT or NOAA surface network observations

This paper compares two global inversions to estimate carbon monoxide (CO) emissions for 2004. Either surface flask observations from the National Oceanic and Atmospheric Administration Earth System Research Laboratory (NOAA/ESRL) Global Monitoring Division (GMD) or CO total columns from the Measurement of Pollution in the Troposphere (MOPITT) instrument are assimilated in a 4D-Var framework. Inferred emission estimates from the two inversions are consistent over the Northern Hemisphere (NH). For example, both inversions increase anthropogenic CO emissions over Europe (from 46 to 94 Tg CO/yr) and Asia (from 222 to 420 Tg CO/yr). In the Southern Hemisphere (SH), three important findings are reported. First, due to their different vertical sensitivity, the stations-only inversion increases SH biomass burning emissions by 108 Tg CO/yr more than the MOPITT-only inversion. Conversely, the MOPITT-only inversion results in SH natural emissions (mainly CO from oxidation of NMVOCs) that are 185 Tg CO/yr higher compared to the stations-only inversion. Second, MOPITT-only derived biomass burning emissions are reduced with respect to the prior which is in contrast to previous (inverse) modeling studies. Finally, MOPITT derived total emissions are significantly higher for South America and Africa compared to the stations-only inversion. This is likely due to a positive bias in the MOPITT V4 product. This bias is also apparent from validation with surface stations and ground-truth FTIR columns. Our results show that a combined inversion is promising in the NH. However, implementation of a satellite bias correction scheme is essential to combine both observational data sets in the SH.

The 2010 Antarctic ozone hole: Observed reduction in ozone destruction by minor sudden stratospheric warmings

Satellite observations show that the 2010 Antarctic ozone hole is characterized by anomalously small amounts of photochemical ozone destruction (40-60% less than the 2005-2009 average). Observations from the MLS instrument show that this is mainly related to reduced photochemical ozone destruction between 20-25 km altitude. Lower down between 15-20 km the atmospheric chemical composition and photochemical ozone destruction is unaffected. The modified chemical composition and chemistry between 20-25 km altitude in 2010 is related to the occurrence of a mid-winter minor Antarctic Sudden Stratospheric Warming (SSW). The measurements indicate that the changes in chemical composition are related to downward motion of air masses rather than horizontal mixing, and affect stratospheric chemistry for several months. Since 1979, years with similar anomalously small amounts of ozone destruction are all characterized by either minor or major SSWs, illustrating that their presence has been a necessary pre-condition for reduced Antarctic stratospheric ozone destruction.

Scanning imaging absorption spectrometer for atmospheric chartography carbon monoxide total columns: statistical evaluation and comparison with chemistry transport model results

This paper presents a detailed statistical analysis of one year (September 2003 to August 2004) of global Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) carbon monoxide (CO) total column retrievals from the Iterative Maximum Likelihood Method (IMLM) algorithm, version 6.3. SCIAMACHY provides the first solar reflectance measurements of CO and is uniquely sensitive down to the boundary layer. SCIAMACHY measurements and chemistry transport model (CTM) results are compared and jointly evaluated. Significant improvements in agreement occur, especially close to biomass burning emission regions, when the new Global Fire Emissions Database version 2 (GFEDv2) is used with the CTM. Globally, the seasonal variation of the model is very similar to that of the SCIAMACHY measurements. For certain locations, significant differences were found, which are likely related to modeling errors due to CO emission uncertainties. Statistical analysis shows that differences between single SCIAMACHY CO total column measurements and corresponding model results are primarily explained by random instrument noise errors. This strongly suggests that the random instrument noise errors are a good diagnostic for the precision of the measurements. The analysis also indicates that noise in single SCIAMACHY CO measurements is generally greater than actual variations in total columns. It is thus required to average SCIAMACHY data over larger temporal and spatial scales to obtain valuable information. Analyses of monthly averaged SCIAMACHY measurements over 3° × 2° geographical regions indicates that they are of sufficient accuracy to reveal valuable information about spatial and temporal variations in CO columns and provide an important tool for model validation. A large spatial and temporal variation in instrument noise errors exists which shows a close correspondence with the spatial distribution of surface albedo and cloud cover. This large spatial variability is important for the use of monthly and annual mean SCIAMACHY CO total column measurements. The smallest instrument noise errors of monthly mean 3° × 2° SCIAMACHY CO total columns measurements are 0.01 × 1018 molecules/cm2 for high surface albedo areas over the Sahara. Errors in SCIAMACHY CO total column retrievals due to errors other than instrument noise, like cloud cover, calibration, retrieval uncertainties and averaging kernels are estimated to be about 0.05–0.1 × 1018 molecules/cm2 in total. The bias found between model and observations is around 0.05–0.1 1018 molecules/cm2 (or about 5%) which also includes model errors. This thus provides a best estimate of the currently achievable measurement accuracy for SCIAMACHY CO monthly mean averages.

Diurnal ozone cycle in the tropical and subtropical marine boundary layer

A conceptual analysis of diurnal ozone (O3) changes in the marine boundary layer (MBL) is presented. Such changes are most pronounced downwind of O3 sources in tropical and subtropical latitudes and during summer at higher latitudes. Previously, it has been assumed that daytime photochemical O3 loss and nighttime replenishment through entrainment from the relatively O3-rich free troposphere explain the diurnal O3 cycle. We show, however, that in a net O3 destruction environment (low NOx) this diurnal cycle can be explained by photochemistry and advection, which establish a horizontal O3 gradient that is typical for the MBL. We support this hypothesis first by calculations with a conceptual one-dimensional (1-D) advection-diffusion model and second by simulations with an interactive 3-D chemistry transport model. The results are in good agreement with observations, for example, in the Indian Ocean Experiment.

EFFECTS OF NEUTRAL HYDROGEN ON COSMIC-RAY PRECURSORS IN SUPERNOVA REMNANT SHOCK WAVES

Many fast supernova remnant shocks show spectra dominated by Balmer lines. The Hα profiles have a narrow component explained by direct excitations and a thermally Doppler broadened component due to atoms that undergo charge exchange in the post-shock region. However, the standard model does not take into account the cosmic-ray shock precursor, which compresses and accelerates plasma ahead of the shock. In strong precursors with sufficiently high densities, the processes of charge exchange, excitation, and ionization will affect the widths of both narrow and broad line components. Moreover, the difference in velocity between the neutrals and the precursor plasma gives rise to frictional heating due to charge exchange and ionization in the precursor. In extreme cases, all neutrals can be ionized by the precursor. In this Letter we compute the ion and electron heating for a wide range of shock parameters, along with the velocity distribution of the neutrals that reach the shock. Our calculations predict very large narrow component widths for some shocks with efficient acceleration, along with changes in the broad-to-narrow intensity ratio used as a diagnostic for the electron-ion temperature ratio. Balmer lines may therefore provide a unique diagnostic of precursor properties. We show that heating by neutrals in the precursor can account for the observed Hα narrow component widths and that the acceleration efficiency is modest in most Balmer line shocks observed thus far.