Modeling lightning-NOx chemistry on a sub-grid scale in a global chemical transport model

For the first time, a plume-in-grid approach is implemented in a chemical transport model (CTM) to parameterize the effects of the nonlinear reactions occurring within high concentrated NO_<i>x</i> plumes from lightning NO_<i>x</i> emissions (LNO_<i>x</i>) in the upper troposphere. It is characterized by a set of parameters including the plume lifetime, the effective reaction rate constant related to NO_<i>x</i>–O₃ chemical interactions, and the fractions of NO_<i>x</i> conversion into HNO₃ within the plume. Parameter estimates were made using the Dynamical Simple Model of Atmospheric Chemical Complexity (DSMACC) box model, simple plume dispersion simulations, and the 3-D Meso-NH (non-hydrostatic mesoscale atmospheric model). In order to assess the impact of the LNO_<i>x</i> plume approach on the NO_<i>x</i> and O₃ distributions on a large scale, simulations for the year 2006 were performed using the GEOS-Chem global model with a horizontal resolution of 2° × 2.5°. The implementation of the LNO_<i>x</i> parameterization implies an NO_<i>x</i> and O₃ decrease on a large scale over the region characterized by a strong lightning activity (up to 25 and 8 %, respectively, over central Africa in July) and a relative increase downwind of LNO_<i>x</i> emissions (up to 18 and 2 % for NO_<i>x</i> and O₃, respectively, in July). The calculated variability in NO_<i>x</i> and O₃ mixing ratios around the mean value according to the known uncertainties in the parameter estimates is at a maximum over continental tropical regions with ΔNO_<i>x</i> [−33.1, +29.7] ppt and ΔO₃ [−1.56, +2.16] ppb, in January, and ΔNO_<i>x</i> [−14.3, +21] ppt and ΔO₃ [−1.18, +1.93] ppb, in July, mainly depending on the determination of the diffusion properties of the atmosphere and the initial NO mixing ratio injected by lightning. This approach allows us (i) to reproduce a more realistic lightning NO_<i>x</i> chemistry leading to better NO_<i>x</i> and O₃ distributions on the large scale and (ii) to focus on other improvements to reduce remaining uncertainties from processes related to NO_<i>x</i> chemistry in CTM

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&amp;deg;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&amp;ndash;14 August 2003), compared to the periods before (16&amp;ndash;31 July 2003) and after (16&amp;ndash;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&amp;times;10&lt;sup&gt;6&lt;/sup&gt; ha in Portugal and added to atmospheric pollution in Europe. Layers with enhanced CO and NO&lt;sub&gt;y&lt;/sub&gt; 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

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

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

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

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&lt;sub&gt;3&lt;/sub&gt;) 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 &amp;minus;25% (except ~5% for MOCAGE) in the case of ozone and from &amp;minus;80% to &amp;minus;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&lt;sub&gt;3&lt;/sub&gt; in this model. Results from sensitivity simulations indicate that an increase of the horizontal resolution to around 1&amp;deg;&amp;times;1&amp;deg; and potential uncertainties in European anthropogenic emissions or in long-range transport of pollution cannot completely account for the underestimation of CO and O&lt;sub&gt;3&lt;/sub&gt; 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

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-3) 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 similar to 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-3 in this model. Results from sensitivity simulations indicate that an increase of the horizontal resolution to around 1 degrees x1 degrees and potential uncertainties in European anthropogenic emissions or in long-range transport of pollution cannot completely account for the underestimation of CO and O-3 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&amp;deg;&amp;times;5&amp;deg; 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&lt;sup&gt;&amp;minus;1&lt;/sup&gt;. 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

Measurements of atmospheric layers from the NASA DC-8 and P-3B aircraft during PEM-Tropics A

Tropospheric vertical structure was analyzed using in situ measurements of O₃, CO, CH₄, and H₂O taken on board the NASA DC-8 aircraft during three Pacific Exploratory Missions (PEMs): PEM-West A, September-October 1991 in the western Pacific; PEM-West B, February-March 1994 in the western Pacific; and PEM-Tropics A, September-October 1996 in the central and eastern Pacific. PEM-Tropics A added measurements from the NASA P3-B aircraft. We used a new mode-based method to define a background against which to find layers. Using only O₃ and H₂O, we found 472 layers in PEM-Tropics A (0.72 layers per vertical kilometer profiled), 237 layers in PEM-West A (0.54 layers/km), and 158 layers in PEM-West B (0.41 layers/km). Using all constituents, we found 187 layers in PEM-Tropics A (0.43 layers/km), 128 layers in PEM-West A (0.29 layers/km), and 80 layers in PEM-West B (0.21 layers/km). Stratospheric air, sometimes mixed with trapped pollution, was the dominant layer source in all three missions. The larger number of layers per kilometer in PEM-Tropics A was probably due to repeated profiling of several “superlayers” visible in many of the mission lidar and potential voracity profiles. The thickness of the superlayers was of order 1 km, and the horizontal extent was of order 1000 km. We found that layers have an important effect on the thermal structure. An example based on ozonesonde data from Tahiti is shown, where a dry, subsiding layer was stabilized by much greater radiative cooling at the base than at the top. The stabilized layer can trap pollution and force vertical plumes to spread into horizontal layers.United States. National Aeronautics and Space Administration (Grant NAG1-1758)United States. National Aeronautics and Space Administration (Grant NAG1-1901