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Lightning is an important natural source of nitrogen oxide especially in the middle and upper troposphere. Hence, it is essential to represent lightning in chemistry transport and coupled chemistry–climate models. Using ERA-Interim meteorological reanalysis data we compare the lightning flash density distributions produced using several existing lightning parametrisations, as well as a new parametrisation developed on the basis of upward cloud ice flux at 440 hPa. The use of ice flux forms a link to the non-inductive charging mechanism of thunderstorms. Spatial and temporal distributions of lightning flash density are compared to tropical and subtropical observations for 2007–2011 from the Lightning Imaging Sensor (LIS) on the Tropical Rainfall Measuring Mission (TRMM) satellite. The well-used lightning flash parametrisation based on cloud-top height has large biases but the derived annual total flash density has a better spatial correlation with the LIS observations than other existing parametrisations. A comparison of flash density simulated by the different schemes shows that the cloud-top height parametrisation has many more instances of moderate flash densities and fewer low and high extremes compared to the other parametrisations. Other studies in the literature have shown that this feature of the cloud-top height parametrisation is in contrast to lightning observations over certain regions. Our new ice flux parametrisation shows a clear improvement over all the existing parametrisations with lower root mean square errors (RMSEs) and better spatial correlations with the observations for distributions of annual total, and seasonal and interannual variations. The greatest improvement with the new parametrisation is a more realistic representation of the zonal distribution with a better balance between tropical and subtropical lightning flash estimates. The new parametrisation is appropriate for testing in chemistry transport and chemistry–climate models that use a lightning parametrisation.

We describe the publicly available data from the Global OZone Chemistry And Related trace gas Data records for the Stratosphere (GOZCARDS) project and provide some results, with a focus on hydrogen chloride (HCl), water vapor (H2O), and ozone (O3). This data set is a global long-term stratospheric Earth system data record, consisting of monthly zonal mean time series starting as early as 1979. The data records are based on high-quality measurements from several NASA satellite instruments and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) on SCISAT. We examine consistency aspects between the various data sets. To merge ozone records, the time series are debiased relative to SAGE II (Stratospheric Aerosol and Gas Experiments) values by calculating average offsets versus SAGE II during measurement overlap periods, whereas for other species the merging derives from an averaging procedure during overlap periods. The GOZCARDS files contain mixing ratios on a common pressure-latitude grid, as well as standard errors and other diagnostics; we also present estimates of systematic uncertainties in the merged products. Monthly mean temperatures for GOZCARDS were also produced, based directly on data from the Modern-Era Retrospective analysis for Research and Applications. The GOZCARDS HCl merged product comes from the Halogen Occultation Experiment (HALOE), ACE-FTS and lower-stratospheric Aura Microwave Limb Sounder (MLS) data. After a rapid rise in upper-stratospheric HCl in the early 1990s, the rate of decrease in this region for 1997-2010 was between 0.4 and 0.7 % yr-1. On 6-8-year timescales, the rate of decrease peaked in 2004-2005 at about 1 % yr-1, and it has since levelled off, at ~ 0.5 % yr-1. With a delay of 6-7 years, these changes roughly follow total surface chlorine, whose behavior versus time arises from inhomogeneous changes in the source gases. Since the late 1990s, HCl decreases in the lower stratosphere have occurred with pronounced latitudinal variability at rates sometimes exceeding 1-2 % yr-1. Recent short-term tendencies of lower-stratospheric and column HCl vary substantially, with increases from 2005 to 2010 for northern midlatitudes and deep tropics, but decreases (increases) after 2011 at northern (southern) midlatitudes. For H2O, the GOZCARDS product covers both stratosphere and mesosphere, and the same instruments as for HCl are used, along with Upper Atmosphere Research Satellite (UARS) MLS stratospheric H2O data (1991-1993). We display seasonal to decadal-type variability in H2O from 22 years of data. In the upper mesosphere, the anticorrelation between H2O and solar flux is now clearly visible over two full solar cycles. Lower-stratospheric tropical H2O has exhibited two periods of increasing values, followed by fairly sharp drops (the well-documented 2000-2001 decrease and a recent drop in 2011-2013). Tropical decadal variability peaks just above the tropopause. Between 1991 and 2013, both in the tropics and on a near-global basis, H2O has decreased by ~ 5-10 % in the lower stratosphere, but about a 10 % increase is observed in the upper stratosphere and lower mesosphere. However, such tendencies may not represent longer-term trends. For ozone, we used SAGE I, SAGE II, HALOE, UARS and Aura MLS, and ACE-FTS data to produce a merged record from late 1979 onward, using SAGE II as the primary reference. Unlike the 2 to 3 % increase in near-global column ozone after the late 1990s reported by some, GOZCARDS stratospheric column O3 values do not show a recent upturn of more than 0.5 to 1 %; long-term interannual column ozone variations from GOZCARDS are generally in very good agreement with interannual changes in merged total column ozone (Version 8.6) data from SBUV instruments. A brief mention is also made of other currently available, commonly formatted GOZCARDS satellite data records for stratospheric composition, namely those for N2O and HNO3.

Vertically resolved distributions of sulfur dioxide (SO2) with global coverage in the height region from the upper troposphere to ~20 km altitude have been derived from observations by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat for the period July 2002 to April 2012. Retrieved volume mixing ratio profiles representing single measurements are characterized by typical errors in the range of 70–100 pptv and by a vertical resolution ranging from 3 to 5 km. Comparison with observations by the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) revealed a slightly varying bias with altitude of −20 to 50 pptv for the MIPAS data set in case of volcanically enhanced concentrations. For background concentrations the comparison showed a systematic difference between the two major MIPAS observation periods. After debiasing, the difference could be reduced to biases within −10 to 20 pptv in the altitude range of 10–20 km with respect to ACE-FTS. Further comparisons of the debiased MIPAS data set with in situ measurements from various aircraft campaigns showed no obvious inconsistencies within a range of around ±50 pptv. The SO2 emissions of more than 30 volcanic eruptions could be identified in the upper troposphere and lower stratosphere (UTLS). Emitted SO2 masses and lifetimes within different altitude ranges in the UTLS have been derived for a large part of these eruptions. Masses are in most cases within estimations derived from other instruments. From three of the major eruptions within the MIPAS measurement period – Kasatochi in August 2008, Sarychev in June 2009 and Nabro in June 2011 – derived lifetimes of SO2 for the altitude ranges 10–14, 14–18 and 18–22 km are 13.3 ± 2.1, 23.6 ± 1.2 and 32.3 ± 5.5 days respectively. By omitting periods with obvious volcanic influence we have derived background mixing ratio distributions of SO2. At 10 km altitude these indicate an annual cycle at northern mid- and high latitudes with maximum values in summer and an amplitude of about 30 pptv. At higher altitudes of about 16–18 km, enhanced mixing ratios of SO2 can be found in the regions of the Asian and the North American monsoons in summer – a possible connection to an aerosol layer discovered by Vernier et al. (2011b) in that region.

We used the GEOS-Chem chemistry-transport model to investigate impacts of surface emissions and dynamical processes on the spatial and temporal patterns of CO observed by the Microwave Limb Sounder (MLS) in the upper troposphere (UT) and lower stratosphere (LS). Model simulations driven by GEOS-4 and GEOS-5 assimilated fields present many features of the seasonal and inter-annual variation of CO in the upper troposphere and lower stratosphere. Both model simulations and the MLS data show a transition from semi-annual variations in the UT to annual variations in the LS. Tagged CO simulations indicate that the semi-annual variation of CO in the UT is determined mainly by the temporal overlapping of surface biomass burning from different continents as well as the north-south shifts of deep convection. Both GEOS-4 and GEOS-5 have maximum upward transport in April and May with a minimum in July to September. The CO peaks from the Northern Hemisphere (NH) fires propagate faster to the LS than do those from the Southern Hemisphere (SH) fires. Thus the transition from a semi-annual to an annual cycle around 80 hPa is induced by a combination of the CO signal at the tropopause and the annual cycle of the Brewer-Dobson circulation. In GEOS-5, the shift to an annual cycle occurs at a lower altitude than in MLS CO, a result of inadequate upward transport. We deduce vertical velocities from MLS CO, and use them to evaluate the velocities derived from the archived GEOS meteorological fields. We find that GEOS-4 velocities are similar to those from MLS CO between 215 hPa and 125 hPa, while the velocities in GEOS-5 are too low in spring and summer. The mean tropical vertical velocities from both models are lower than those inferred from MLS CO above 100 hPa, particularly in GEOS-5, with mean downward, rather than upward motion in boreal summer. Thus the models' CO maxima from SH burning are transported less effectively than those in MLS CO above 147 hPa and almost disappear by 100 hPa. The strongest peaks in the CO tape-recorder are in late 2004, 2006, and 2010, with the first two resulting from major fires in Indonesia and the last from severe burning in South America, all associated with intense droughts.

Variations in the mixing ratio of long‐lived trace gases entering the stratosphere in the tropics are carried upward with the rising air with the signal being observable throughout the tropical lower stratosphere. This phenomenon, referred to as “atmospheric tape recorder” has previously been observed for water vapor, CO2, and CO which exhibit an annual cycle. Recently, based on Microwave Limb Sounder (MLS) and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE‐FTS) satellite measurements, the tape recorder signal has been observed for hydrogen cyanide (HCN) but with an approximately two‐year period. Here we report on a model simulation of the HCN tape recorder for the time period 2002–2008 using the Chemical Lagrangian Model of the Stratosphere (CLaMS). The model can reproduce the observed pattern of the HCN tape recorder signal if time‐resolved emissions from fires in Indonesia are used as lower boundary condition. This finding indicates that inter‐annual variations in biomass burning in Indonesia, which are strongly influenced by El Niño events, control the HCN tape recorder signal. A longer time series of tropical HCN data will probably exhibit an irregular cycle rather than a regular biannual cycle.

The large bush fires which occurred in southeast Australia in February 2009 were unusually destructive. However, they were also unusual in the amounts of various combustion products which were injected directly into the stratosphere. We report the observations by the Microwave Limb Sounder (MLS) instrument on the Aura satellite of some of these combustion products. The highest quality observations are of CO; these clearly show a large region of enhanced mixing ratios to the north of New Zealand which remains in that region for about ten days before drifting westwards and finally dissipating over the Atlantic about a month after the fire. The region of enhanced CO ascends from the tropopause to 46 hPa during this period. Back trajectories run from the points where MLS observes enhanced CO pass close to the site of the fire. The MLS observations of CH3CN and HCN resemble those of CO except for their poorer vertical resolution and more limited vertical range. An apparent enhancement in ClO is also observed by MLS, but detailed analysis of the measured radiances reveals this feature to be a signature of CH3OH, which is not currently retrieved by the MLS data processing system. The fires of February 2009 are the only event of this type and magnitude in the 7-yr MLS record.

The photochemical production and loss rates for carbon monoxide (CO) in the stratosphere and mesosphere are evaluated using measurements from the Aura Microwave Limb Sounder (MLS) and the Atmospheric Chemistry Experiment‐Fourier Transform Spectrometer (ACE‐FTS). The distributions of reactive trace gases involved in the photochemistry of CO, including OH, CH4, O(1D), Cl, as well as temperatures for calculating reaction rates, are either directly observed or constrained from observations. We map the CO net production and loss as a function of pressure (10–0.02 hPa, about 30–75 km altitude), latitude (approximately ±70°), and season. The results indicate that photochemical loss dominates over production for nearly all conditions considered here. A minimum photochemical loss lifetime of about 10 days occurs near the 2 hPa pressure level, and it follows the region of maximum sunlight exposure. At high latitudes during winter, the CO lifetime is generally longer than 30 days. Time scales become much shorter in spring, however, when CO lifetimes can be 15–20 days poleward of 60° latitude in the upper stratosphere. On the basis of these results, CO is a suitable tracer during autumn to spring above the 0.1 hPa pressure level but not in the upper stratosphere near 1 hPa.

Upper Atmosphere Research Satellite observations indicate that extensive denitrification without significant dehydration currently occurs only in the Antarctic during mid to late June. The fact that denitrification occurs in a relatively warm month in the Antarctic raises concern about the likelihood of its occurrence and associated effects on ozone recovery in a colder and possibly more humid future Arctic lower stratosphere. Polar stratospheric cloud lifetimes required for Arctic denitrification to occur in the future are presented and contrasted against the current Antarctic cloud lifetimes. Model calculations show that widespread severe denitrification could enhance future Arctic ozone loss by up to 30%.

This paper presents an evaluation of a new linear parameterization valid for the troposphere and the stratosphere, based on a first order approximation of the carbon monoxide (CO) continuity equation. This linear scheme (hereinafter noted LINCO) has been implemented in the 3-D Chemical Transport Model (CTM) MOCAGE (MOdèle de Chimie Atmospherique Grande Echelle). First, a one and a half years of LINCO simulation has been compared to output obtained from a detailed chemical scheme output. The mean differences between both schemes are about ±25 ppbv (part per billion by volume) or 15% in the troposphere and ±10 ppbv or 100% in the stratosphere. Second, LINCO has been compared to diverse observations from satellite instruments covering the troposphere (Measurements Of Pollution In The Troposphere: MOPITT) and the stratosphere (Microwave Limb Sounder: MLS) and also from aircraft (Measurements of ozone and water vapour by Airbus in-service aircraft: MOZAIC programme) mostly flying in the upper troposphere and lower stratosphere (UTLS). In the troposphere, the LINCO seasonal variations as well as the vertical and horizontal distributions are quite close to MOPITT CO observations. However, a bias of ~−40 ppbv is observed at 700 Pa between LINCO and MOPITT. In the stratosphere, MLS and LINCO present similar large-scale patterns, except over the poles where the CO concentration is underestimated by the model. In the UTLS, LINCO presents small biases less than 2% compared to independent MOZAIC profiles. Third, we assimilated MOPITT CO using a variational 3D-FGAT (First Guess at Appropriate Time) method in conjunction with MOCAGE for a long run of one and a half years. The data assimilation greatly improves the vertical CO distribution in the troposphere from 700 to 350 hPa compared to independent MOZAIC profiles. At 146 hPa, the assimilated CO distribution is also improved compared to MLS observations by reducing the bias up to a factor of 2 in the tropics. This study confirms that the linear scheme is able to simulate reasonably well the CO distribution in the troposphere and in the lower stratosphere. Therefore, the low computing cost of the linear scheme opens new perspectives to make free runs and CO data assimilation runs at high resolution and over periods of several years.

A space shuttle launch deposits 700 tonnes of water in the atmosphere. Some of this water is released into the upper mesosphere and lower thermosphere where it may be directly detected by a limb sounding satellite instrument. We report measurements of water vapour plumes from shuttle launches made by the Microwave Limb Sounder (MLS) on the Aura satellite. Approximately 50%–65% of shuttle launches are detected by MLS. The signal appears at a similar level across the upper 10 km of the MLS limb scan, suggesting that the bulk of the observed water is above the top of the scan. Only a small fraction at best of smaller launches (Ariane 5, Proton) are detected. We conclude that the sensitivity of MLS is only just great enough to detect a shuttle sized launch, but that a suitably designed instrument of the same general type could detect the exhausts from a large proportion of heavy-lift launches.