The influence of biogenic emissions from Africa on tropical tropospheric ozone during 2006: a global modeling study

We have performed simulations using a 3-D global chemistry-transport model to investigate the influence that biogenic emissions from the African continent exert on the composition of the troposphere in the tropical region. For this purpose we have applied two recently developed biogenic emission inventories provided for use in large-scale global models (Granier et al., 2005; LathiSre et al., 2006) whose seasonality and temporal distribution for biogenic emissions of isoprene, other volatile organic compounds and NO is markedly different. The use of the 12 year average values for biogenic emissions provided by LathiSre et al. (2006) results in an increase in the amount of nitrogen sequestrated into longer lived reservoir compounds which contributes to the reduction in the tropospheric ozone burden in the tropics. The associated re-partitioning of nitrogen between PAN, HNO3 and organic nitrates also results in a similar to 5% increase in the loss of nitrogen by wet deposition. At a global scale there is a reduction in the oxidizing capacity of the model atmosphere which increases the atmospheric lifetimes of CH4 and CO by similar to 1.5% and similar to 4%, respectively. Comparisons against a range of different measurements indicate that applying the 12 year average of LathiSre et al. (2006) improves the performance of TM4_AMMA for 2006 in the tropics. By the use of sensitivity studies we show that the release of NO from soils in Africa accounts for between similar to 2-45% of tropospheric ozone in the African troposphere, similar to 10% in the upper troposphere and between similar to 5-20% of the tropical tropospheric ozone column over the tropical Atlantic Ocean. The subsequent reduction in OH over the source regions allows enhanced transport of CO out of the region. For biogenic volatile organic C1 to C3 species released from Africa, the effects on tropical tropospheric ozone are rather limited, although this source contributes to the global burden of VOC by between similar to 2-4% and has a large influence on the organic composition of the troposphere over the tropical Atlantic Ocean

Air pollution during the 2003 European heat wave as seen by MOZAIC airliners

This study presents an analysis of both MOZAIC profiles above Frankfurt and Lagrangian dispersion model simulations for the 2003 European heat wave. The comparison of MOZAIC measurements in summer 2003 with the 11-year MOZAIC climatology reflects strong temperature anomalies (exceeding 4°C) throughout the lower troposphere. Higher positive anomalies of temperature and negative anomalies of both wind speed and relative humidity are found for the period defined here as the heat wave (2–14 August 2003), compared to the periods before (16–31 July 2003) and after (16–31 August 2003) the heat wave. In addition, Lagrangian model simulations in backward mode indicate the suppressed long-range transport in the mid- to lower troposphere and the enhanced southern origin of air masses for all tropospheric levels during the heat wave. Ozone and carbon monoxide also present strong anomalies (both ~+40 ppbv) during the heat wave, with a maximum vertical extension reaching 6 km altitude around 11 August 2003. Pollution in the planetary boundary layer (PBL) is enhanced during the day, with ozone mixing ratios two times higher than climatological values. This is due to a combination of factors, such as high temperature and radiation, stagnation of air masses and weak dry deposition, which favour the accumulation of ozone precursors and the build-up of ozone. A negligible role of a stratospheric-origin ozone tracer has been found for the lower troposphere in this study. From 29 July to 15 August 2003 forest fires burnt around 0.3×10<sup>6</sup> ha in Portugal and added to atmospheric pollution in Europe. Layers with enhanced CO and NO<sub>y</sub> mixing ratios, advected from Portugal, were crossed by the MOZAIC aircraft in the free troposphere over Frankfurt. A series of forward and backward Lagrangian model simulations have been performed to investigate the origin of anomalies during the whole heat wave. European anthropogenic emissions present the strongest contribution to the measured CO levels in the lower troposphere (near 30%). This source is followed by Portuguese forest fires which affect the lower troposphere after 6 August 2003 and even the PBL around 10 August 2003. The averaged biomass burning contribution reaches 35% during the affected period. Anthropogenic CO of North American origin only marginally influences CO levels over Europe during that period

the Creative Commons Attribution 3.0 License. Atmospheric Chemistry and Physics

The influence of biogenic emissions from Africa on tropical tropospheric ozone during 2006: a global modeling stud

A conscious rethink : Why is brain tissue commonly preserved in the archaeological record? Commentary on: Petrone P, Pucci P, Niola M, et al. Heat-induced brain vitrification from the Vesuvius eruption in C.E. 79. N Engl J Med 2020;382:383-4. DOI: 10.1056/NEJMc1909867

Brain tissue is ubiquitous in the archaeological record. Multiple, independent studies report the finding of black, resinous or shiny brain tissue, and Petrone et al. [2020 “Heat-induced Brain Vitrification from the Vesuvius Eruption in C.E. 79.” N Engl J Med. 382: 383–384; doi:10.1056/NEJMc1909867] raise the intriguing prospect of a role for vitrification in the preservation of ancient biomolecules. However, Petrone et al. (2020) have not made their raw data available, and no detailed laboratory or analytical methodology is offered. Issues of contamination and misinterpretation hampered a decade of research in biomolecular archaeology, such that addressing these sources of bias and facilitating validation of specious findings has become both routine and of paramount importance in the discipline. We argue that the evidence they present does not support their conclusion of heat-induced vitrification of human brain tissue, and that future studies should share palaeoproteomic data in an open access repository to facilitate comparative analysis of the recovery of ancient proteins and patterns of their degradation

Comprehensive evaluation of the Copernicus Atmosphere Monitoring Service (CAMS) reanalysis against independent observations: Reactive gases

The Copernicus Atmosphere Monitoring Service (CAMS) is operationally providing forecast and reanalysis products of air quality and atmospheric composition. In this article, we present an extended evaluation of the CAMS global reanalysis data set of four reactive gases, namely, ozone (O-3), carbon monoxide (CO), nitrogen dioxide (NO2), and formaldehyde (HCHO), using multiple independent observations. Our results show that the CAMS model system mostly provides a stable and accurate representation of the global distribution of reactive gases over time. Our findings highlight the crucial impact of satellite data assimilation and emissions, investigated through comparison with a model run without assimilated data. Stratospheric and tropospheric O-3 are mostly well constrained by the data assimilation, except over Antarctica after 2012/2013 due to changes in the assimilated data. Challenges remain for O-3 in the Tropics and high-latitude regions during winter and spring. At the surface and for short-lived species (NO2), data assimilation is less effective. Total column CO in the CAMS reanalysis is well constrained by the assimilated satellite data. The control run, however, shows large overestimations of total column CO in the Southern Hemisphere and larger year-to-year variability in all regions. Concerning the long-term stability of the CAMS model, we note drifts in the time series of biases for surface O-3 and CO in the Northern midlatitudes and Tropics and for NO2 over East Asia, which point to biased emissions. Compared to the previous Monitoring Atmospheric Composition and Climate reanalysis, changes in the CAMS chemistry module and assimilation system helped to reduce biases and enhance the long-term temporal consistency of model results for the CAMS reanalysis

Global model simulations of air pollution during the 2003 European heat wave

Three global Chemistry Transport Models – MOZART, MOCAGE, and TM5 – as well as MOZART coupled to the IFS meteorological model including assimilation of ozone (O<sub>3</sub>) and carbon monoxide (CO) satellite column retrievals, have been compared to surface measurements and MOZAIC vertical profiles in the troposphere over Western/Central Europe for summer 2003. The models reproduce the meteorological features and enhancement of pollution during the period 2–14 August, but not fully the ozone and CO mixing ratios measured during that episode. Modified normalised mean biases are around −25% (except ~5% for MOCAGE) in the case of ozone and from −80% to −30% for CO in the boundary layer above Frankfurt. The coupling and assimilation of CO columns from MOPITT overcomes some of the deficiencies in the treatment of transport, chemistry and emissions in MOZART, reducing the negative biases to around 20%. The high reactivity and small dry deposition velocities in MOCAGE seem to be responsible for the overestimation of O<sub>3</sub> in this model. Results from sensitivity simulations indicate that an increase of the horizontal resolution to around 1°×1° and potential uncertainties in European anthropogenic emissions or in long-range transport of pollution cannot completely account for the underestimation of CO and O<sub>3</sub> found for most models. A process-oriented TM5 sensitivity simulation where soil wetness was reduced results in a decrease in dry deposition fluxes and a subsequent ozone increase larger than the ozone changes due to the previous sensitivity runs. However this latest simulation still underestimates ozone during the heat wave and overestimates it outside that period. Most probably, a combination of the mentioned factors together with underrepresented biogenic emissions in the models, uncertainties in the modelling of vertical/horizontal transport processes in the proximity of the boundary layer as well as limitations of the chemistry schemes are responsible for the underestimation of ozone (overestimation in the case of MOCAGE) and CO found in the models during this extreme pollution event

Validation of Aura Microwave Limb Sounder O-3 and CO observations in the upper troposphere and lower stratosphere

International audienceGlobal satellite observations of ozone and carbon monoxide from the Microwave Limb Sounder (MLS) on the EOS Aura spacecraft are discussed with emphasis on those observations in the 215–100 hPa region (the upper troposphere and lower stratosphere). The precision, resolution and accuracy of the data produced by the MLS “version 2.2” processing algorithms are discussed and quantified. O3 accuracy is estimated at ~40 ppbv +5% (~20 ppbv +20% at 215 hPa) while the CO accuracy is estimated at ~30 ppbv +30% for pressures of 147 hPa and less. Comparisons with expectations and other observations show good agreements for the O3 product, generally consistent with the systematic errors quoted above. In the case of CO, a persistent factor of ~2 high bias is seen at 215 hPa. However, the morphology is shown to be realistic, consistent with raw MLS radiance data, and useful for scientific study. The MLS CO data at higher altitudes are shown to be consistent with other observations

Global estimates of CO sources with high resolution by adjoint inversion of multiple satellite datasets (MOPITT, AIRS, SCIAMACHY, TES)

We combine CO column measurements from the MOPITT, AIRS, SCIAMACHY, and TES satellite instruments in a full-year (May 2004–April 2005) global inversion of CO sources at 4°×5° spatial resolution and monthly temporal resolution. The inversion uses the GEOS-Chem chemical transport model (CTM) and its adjoint applied to MOPITT, AIRS, and SCIAMACHY. Observations from TES, surface sites (NOAA/GMD), and aircraft (MOZAIC) are used for evaluation of the a posteriori solution. Using GEOS-Chem as a common intercomparison platform shows global consistency between the different satellite datasets and with the in situ data. Differences can be largely explained by different averaging kernels and a priori information. The global CO emission from combustion as constrained in the inversion is 1350 Tg a<sup>−1</sup>. This is much higher than current bottom-up emission inventories. A large fraction of the correction results from a seasonal underestimate of CO sources at northern mid-latitudes in winter and suggests a larger-than-expected CO source from vehicle cold starts and residential heating. Implementing this seasonal variation of emissions solves the long-standing problem of models underestimating CO in the northern extratropics in winter-spring. A posteriori emissions also indicate a general underestimation of biomass burning in the GFED2 inventory. However, the tropical biomass burning constraints are not quantitatively consistent across the different datasets

Interpretation of TOMS observations of tropical tropospheric ozone with a global model and in-situ observations

We interpret the distribution of tropical tropospheric ozone columns (TTOCs) from the Total Ozone Mapping Spectrometer (TOMS) by using a global three-dimensional model of tropospheric chemistry (GEOS-CHEM) and additional information from in situ observations. The GEOS-CHEM TTOCs capture 44% of the variance of monthly mean TOMS TTOCs from the convective cloud differential method (CCD) with no global bias. Major discrepancies are found over northern Africa and south Asia where the TOMS TTOCs do not capture the seasonal enhancements from biomass burning found in the model and in aircraft observations. A characteristic feature of these northern tropical enhancements, in contrast to southern tropical enhancements, is that they are driven by the lower troposphere where the sensitivity of TOMS is poor due to Rayleigh scattering. We develop an efficiency correction to the TOMS retrieval algorithm that accounts for the variability of ozone in the lower troposphere. This efficiency correction increases TTOCs over biomass burning regions by 3–5 Dobson units (DU) and decreases them by 2–5 DU over oceanic regions, improving the agreement between CCD TTOCs and in situ observations. Applying the correction to CCD TTOCs reduces by ∼5 DU the magnitude of the “tropical Atlantic paradox” [Thompson et al., 2000], i.e. the presence of a TTOC enhancement over the southern tropical Atlantic during the northern African biomass burning season in December–February. We reproduce the remainder of the paradox in the model and explain it by the combination of upper tropospheric ozone production from lightning NOx, persistent subsidence over the southern tropical Atlantic as part of the Walker circulation, and cross-equatorial transport of upper tropospheric ozone from northern midlatitudes in the African “westerly duct.” These processes in the model can also account for the observed 13–17 DU persistent wave-1 pattern in TTOCs with a maximum over the tropical Atlantic and a minimum over the tropical Pacific during all seasons. The photochemical effects of mineral dust have only a minor role on the modeled distribution of TTOCs, including over northern Africa, due to multiple competing effects. The photochemical effects of mineral dust globally decrease annual mean OH concentrations by 9%. A global lightning NOx source of 6 Tg N yr−1 in the model produces a simulation that is most consistent with TOMS and in situ observations