Cross-tropopause Transport Research Articles

Analysis of the global atmospheric background sulfur budget in a multi-model framework

Abstract. A growing number of general circulation models are adapting interactive sulfur and aerosol schemes to improve the representation of relevant physical and chemical processes and associated feedbacks. They are motivated by investigations of climate response to major volcanic eruptions and potential solar geoengineering scenarios. However, uncertainties in these schemes are not well constrained. Stratospheric sulfate is modulated by emissions of sulfur-containing species of anthropogenic and natural origin, including volcanic activity. While the effects of volcanic eruptions have been studied in the framework of global model intercomparisons, the background conditions of the sulfur cycle have not been addressed in such a way. Here, we fill this gap by analyzing the distribution of the main sulfur species in nine global atmospheric aerosol models for a volcanically quiescent period. We use observational data to evaluate model results. Overall, models agree that the three dominant sulfur species in terms of burdens (sulfate aerosol, OCS, and SO2) make up about 98 % stratospheric sulfur and 95 % tropospheric sulfur. However, models vary considerably in the partitioning between these species. Models agree that anthropogenic emission of SO2 strongly affects the sulfate aerosol burden in the northern hemispheric troposphere, while its importance is very uncertain in other regions, where emissions are much lower. Sulfate aerosol is the main deposited species in all models, but the values deviate by a factor of 2. Additionally, the partitioning between wet and dry deposition fluxes is highly model dependent. Inter-model variability in the sulfur species is low in the tropics and increases towards the poles. Differences are largest in the dynamically active northern hemispheric extratropical region and could be attributed to the representation of the stratospheric circulation. The differences in the atmospheric sulfur budget among the models arise from the representation of both chemical and dynamical processes, whose interplay complicates the bias attribution. Several problematic points identified for individual models are related to the specifics of the chemistry schemes, model resolution, and representation of cross-tropopause transport in the extratropics. Further model intercomparison research is needed with a focus on the clarification of the reasons for biases, given the importance of this topic for the stratospheric aerosol injection studies.

Evaluation of modelled climatologies of O3, CO, water vapour and NOy in the upper troposphere–lower stratosphere using regular in situ observations by passenger aircraft

Abstract. Evaluating global chemistry models in the upper troposphere–lower stratosphere (UTLS) is an important step toward an improved understanding of the chemical composition in this region. This composition is regularly sampled through in situ measurements based on passenger aircraft, in the framework of the In-service Aircraft for a Global Observing System (IAGOS) research infrastructure. This study focuses on the comparison of the IAGOS measurements in ozone, carbon monoxide (CO), nitrogen reactive species (NOy) and water vapour, with a 25-year simulation output from the LMDZ-OR-INCA chemistry–climate model. For this purpose, we present and apply an extension of the Interpol-IAGOS software that projects the IAGOS data onto any model grid, in order to derive a gridded IAGOS product and a masked (sub-sampled) model product that are directly comparable to one another. Climatologies are calculated in the upper troposphere (UT) and in the lower stratosphere (LS) separately but also in the UTLS as a whole, as a demonstration for the models that do not sort out the physical variables necessary to distinguish between the UT and the LS. In the northern extratropics, the comparison in the UTLS layer suggests that the geographical distribution in the tropopause height is well reproduced by the model. In the separated layers, the model simulates well the water vapour climatologies in the UT and the ozone climatologies in the LS. There are opposite biases in CO in both UT and LS, which suggests that the cross-tropopause transport is overestimated. The NOy observations highlight the difficulty of the model in parameterizing the lightning emissions. In the tropics, the upper-tropospheric climatologies are remarkably well simulated for water vapour. They also show realistic CO peaks due to biomass burning in the most convective systems, and the ozone latitudinal variations are well correlated between the observations and the model. Ozone is more sensitive to lightning emissions than to biomass burning emissions, whereas the CO sensitivity to biomass burning emissions strongly depends on location and season. The present study demonstrates that the Interpol-IAGOS software is a tool facilitating the assessment of global model simulations in the UTLS, which is potentially useful for any modelling experiment involving chemistry climate or chemistry transport models.

Mean age from observations in the lowermost stratosphere: an improved method and interhemispheric differences

Abstract. The age of stratospheric air is a concept commonly used to evaluate transport timescales in atmospheric models. The mean age can be derived from observations of a single long-lived trace gas species with a known tropospheric trend. Commonly, deriving mean age is based on the assumption that all air enters the stratosphere through the tropical (TR) tropopause. However, in the lowermost stratosphere (LMS) close to the extra-tropical (exTR) tropopause, cross-tropopause transport needs to be taken into account. We introduce the new exTR–TR method, which considers exTR input into the stratosphere in addition to TR input. We apply the exTR–TR method to in situ SF6 measurements from three aircraft campaigns (PGS, WISE and SouthTRAC) and compare results to those from the conventional TR-only method. Using the TR-only method, negative mean age values are derived in the LMS close to the tropopause during the WISE campaign in Northern Hemispheric (NH) fall 2017. Using the new exTR–TR method instead, the number and extent of negative mean age values is reduced. With our new exTR–TR method, we are thus able to derive more realistic values of typical transport times in the LMS from in situ SF6 measurements. Absolute differences between both methods range from 0.3 to 0.4 years among the three campaigns. Interhemispheric differences in mean age are found when comparing seasonally overlapping campaign phases from the PGS and the SouthTRAC campaigns. On average, within the lowest 65 K potential temperature above the tropopause, the NH LMS is 0.5±0.3 years older around March 2016 than the Southern Hemispheric (SH) LMS around September 2019. The derived differences between results from the exTR–TR method and the TR-only method, as well as interhemispheric differences, are higher than the sensitivities of the exTR–TR method to parameter uncertainties, which are estimated to be below 0.22 years for all three campaigns.

Cross-Tropopause Transport of Surface Pollutants during the Beijing 21 July Deep Convection Event

Abstract Air transport from the troposphere to the stratosphere plays an important role in altering the vertical distribution of pollutants in the upper troposphere and lower stratosphere (UTLS). On 21 July 2012, Beijing was hit by an unprecedented extreme rainfall event. In the present study, the Community Multiscale Air Quality Modeling System (CMAQ) is used to simulate the change in vertical profiles of pollutants during this event. The integrated process rate (IPR) method was applied to quantify the relative contributions from different atmospheric processes to the changes in the vertical profile of pollutants and to estimate the vertical transport flux across the tropopause. The results revealed that, in the tropopause layer, during the torrential rainfall event, the values of O3 decreased by 35% and that of CO increased by 98%, while those of SO2, NO2, and PM2.5 increased slightly. Atmospheric transport was the main cause for the change in O3 values, contributing 32% of the net increase and 99% of the net decrease of O3. The calculations showed that the transport masses of CO, O3, PM2.5, NO2, and SO2 to the stratosphere by this deep convection in 25 h were 6.0 × 107, 2.4 × 107, 7.9 × 105, 2.2 × 105, and 2.7 × 103 kg, respectively, within the ∼300 km × 300 km domain. In the midlatitudes of the Northern Hemisphere, penetrating deep convective activities can transport boundary layer pollutants into the UTLS layer, which will have a significant impact on the climate of this layer.

On the cross-tropopause transport of water by tropical convective overshoots: a mesoscale modelling study constrained by in situ observations during the TRO-Pico field campaign in Brazil

Abstract. Deep convection overshooting the lowermost stratosphere is well known for its role in the local stratospheric water vapour (WV) budget. While it is seldom the case, local enhancement of WV associated with stratospheric overshoots is often published. Nevertheless, one debatable topic persists regarding the global impact of this event with respect to the temperature-driven dehydration of air parcels entering the stratosphere. As a first step, it is critical to quantify their role at a cloud-resolving scale before assessing their impact on a large scale in a climate model. It would lead to a nudging scheme for large-scale simulation of overshoots. This paper reports on the local enhancements of WV linked to stratospheric overshoots, observed during the TRO-Pico campaign conducted in March 2012 in Bauru, Brazil, using the BRAMS (Brazilian version of the Regional Atmospheric Modeling System; RAMS) mesoscale model. Since numerical simulations depend on the choice of several preferred parameters, each having its uncertainties, we vary the microphysics or the vertical resolution while simulating the overshoots. Thus, we produce a set of simulations illustrating the possible variations in representing the stratospheric overshoots. To better resolve the stratospheric hydration, we opt for simulations with the 800 m horizontal-grid-point presentation. Next, we validate these simulations against the Bauru S-band radar echo tops and the TRO-Pico balloon-borne observations of WV and particles. Two of the three simulations' setups yield results compatible with the TRO-Pico observations. From these two simulations, we determine approximately 333–2000 t of WV mass prevailing in the stratosphere due to an overshooting plume depending on the simulation setup. About 70 % of the ice mass remains between the 380 and 385 K isentropic levels. The overshooting top comprises pristine ice and snow, while aggregates only play a role just above the tropopause. Interestingly, the horizontal cross section of the overshooting top is about 450 km2 at the 380 K isentrope, which is similar to the horizontal-grid-point resolution of a simulation that cannot compute overshoots explicitly. In a large-scale simulation, these findings could provide guidance for a nudging scheme of overshooting hydration or dehydration.

Enhanced stratospheric intrusion at Lulin Mountain, Taiwan inferred from beryllium-7 activity

Beryllium-7 (7Be), produced by the interaction of cosmic radiation with atoms and molecules primarily in the upper troposphere and lower stratosphere, provides a useful tracer of cross-tropopause transport and vertical mixing in the troposphere. In the western Pacific subtropical region, the interaction of the subtropical jet stream with monsoon systems potentially enhances the transport. Here, we report one year of 7Be measurements at daily resolution during 2010, at Mt. Lulin (2862 m above mean sea level; NOAA code: LLN), along with other gaseous compounds such as O3 and CO and meteorological information, to assess processes that affect the variability of 7Be. The 7Be concentrations are of the order 1 mBq/m3 or less. The 7Be activity is generally low during summer, largely due to precipitation and unfavorable conditions of atmospheric dynamics (i.e., prevalence of upward motion), but it is occasionally high because of the influence of typhoons. In winter and spring, stratospheric effects observed at the surface were frequent and significant, thereby directly affecting the strength of stratospheric effects on the troposphere, such as the tropospheric oxidation capacity. The effects of the stratospheric intrusions are seen by negative and positive correlations of 7Be with relative humidity and concentration of O3, respectively. The stratospheric effect is further supported by the presence of downwelling transport in this region in the European Centre for Medium-Range Weather Forecasts-Atmospheric Composition Reanalysis Version 4 CO, O3, and relative humidity data.

Impact of Lagrangian transport on lower-stratospheric transport timescales in a climate model

Abstract. We investigate the impact of model trace gas transport schemes on the representation of transport processes in the upper troposphere and lower stratosphere. Towards this end, the Chemical Lagrangian Model of the Stratosphere (CLaMS) was coupled to the ECHAM/MESSy Atmospheric Chemistry (EMAC) model and results from the two transport schemes (Lagrangian critical Lyapunov scheme and flux-form semi-Lagrangian, respectively) were compared. Advection in CLaMS was driven by the EMAC simulation winds, and thereby the only differences in transport between the two sets of results were caused by differences in the transport schemes. To analyze the timescales of large-scale transport, multiple tropical-surface-emitted tracer pulses were performed to calculate age of air spectra, while smaller-scale transport was analyzed via idealized, radioactively decaying tracers emitted in smaller regions (nine grid cells) within the stratosphere. The results show that stratospheric transport barriers are significantly stronger for Lagrangian EMAC-CLaMS transport due to reduced numerical diffusion. In particular, stronger tracer gradients emerge around the polar vortex, at the subtropical jets, and at the edge of the tropical pipe. Inside the polar vortex, the more diffusive EMAC flux-form semi-Lagrangian transport scheme results in a substantially higher amount of air with ages from 0 to 2 years (up to a factor of 5 higher). In the lowermost stratosphere, mean age of air is much smaller in EMAC, owing to stronger diffusive cross-tropopause transport. Conversely, EMAC-CLaMS shows a summertime lowermost stratosphere age inversion – a layer of older air residing below younger air (an “eave”). This pattern is caused by strong poleward transport above the subtropical jet and is entirely blurred by diffusive cross-tropopause transport in EMAC. Potential consequences from the choice of the transport scheme on chemistry–climate and geoengineering simulations are discussed.

Improved tropospheric and stratospheric sulfur cycle in the aerosol–chemistry–climate model SOCOL-AERv2

Abstract. SOCOL-AERv1 was developed as an aerosol–chemistry–climate model to study the stratospheric sulfur cycle and its influence on climate and the ozone layer. It includes a sectional aerosol model that tracks the sulfate particle size distribution in 40 size bins, between 0.39 nm and 3.2 µm. Sheng et al. (2015) showed that SOCOL-AERv1 successfully matched observable quantities related to stratospheric aerosol. In the meantime, SOCOL-AER has undergone significant improvements and more observational datasets have become available. In producing SOCOL-AERv2 we have implemented several updates to the model: adding interactive deposition schemes, improving the sulfate mass and particle number conservation, and expanding the tropospheric chemistry scheme. We compare the two versions of the model with background stratospheric sulfate aerosol observations, stratospheric aerosol evolution after Pinatubo, and ground-based sulfur deposition networks. SOCOL-AERv2 shows similar levels of agreement as SOCOL-AERv1 with satellite-measured extinctions and in situ optical particle counter (OPC) balloon flights. The volcanically quiescent total stratospheric aerosol burden simulated in SOCOL-AERv2 has increased from 109 Gg of sulfur (S) to 160 Gg S, matching the newly available satellite estimate of 165 Gg S. However, SOCOL-AERv2 simulates too high cross-tropopause transport of tropospheric SO2 and/or sulfate aerosol, leading to an overestimation of lower stratospheric aerosol. Due to the current lack of upper tropospheric SO2 measurements and the neglect of organic aerosol in the model, the lower stratospheric bias of SOCOL-AERv2 was not further improved. Model performance under volcanically perturbed conditions has also undergone some changes, resulting in a slightly shorter volcanic aerosol lifetime after the Pinatubo eruption. With the improved deposition schemes of SOCOL-AERv2, simulated sulfur wet deposition fluxes are within a factor of 2 of measured deposition fluxes at 78 % of the measurement stations globally, an agreement which is on par with previous model intercomparison studies. Because of these improvements, SOCOL-AERv2 will be better suited to studying changes in atmospheric sulfur deposition due to variations in climate and emissions.

Sixty years of radiocarbon dioxide measurements at Wellington, New Zealand: 1954–2014

Abstract. We present 60 years of Δ14CO2 measurements from Wellington, New Zealand (41° S, 175° E). The record has been extended and fully revised. New measurements have been used to evaluate the existing record and to replace original measurements where warranted. This is the earliest direct atmospheric Δ14CO2 record and records the rise of the 14C bomb spike and the subsequent decline in Δ14CO2 as bomb 14C moved throughout the carbon cycle and increasing fossil fuel CO2 emissions further decreased atmospheric Δ14CO2. The initially large seasonal cycle in the 1960s reduces in amplitude and eventually reverses in phase, resulting in a small seasonal cycle of about 2 ‰ in the 2000s. The seasonal cycle at Wellington is dominated by the seasonality of cross-tropopause transport and differs slightly from that at Cape Grim, Australia, which is influenced by anthropogenic sources in winter. Δ14CO2 at Cape Grim and Wellington show very similar trends, with significant differences only during periods of known measurement uncertainty. In contrast, similar clean-air sites in the Northern Hemisphere show a higher and earlier bomb 14C peak, consistent with a 1.4-year interhemispheric exchange time. From the 1970s until the early 2000s, the Northern and Southern Hemisphere Δ14CO2 were quite similar, apparently due to the balance of 14C-free fossil fuel CO2 emissions in the north and 14C-depleted ocean upwelling in the south. The Southern Hemisphere sites have shown a consistent and marked elevation above the Northern Hemisphere sites since the early 2000s, which is most likely due to reduced upwelling of 14C-depleted and carbon-rich deep waters in the Southern Ocean, although an underestimate of fossil fuel CO2 emissions or changes in biospheric exchange are also possible explanations. This developing Δ14CO2 interhemispheric gradient is consistent with recent studies that indicate a reinvigorated Southern Ocean carbon sink since the mid-2000s and suggests that the upwelling of deep waters plays an important role in this change.

Quantifying pollution transport from the Asian monsoon anticyclone into the lower stratosphere

Abstract. Pollution transport from the surface to the stratosphere within the Asian monsoon circulation may cause harmful effects on stratospheric chemistry and climate. Here, we investigate air mass transport from the monsoon anticyclone into the stratosphere using a Lagrangian chemistry transport model. We show how two main transport pathways from the anticyclone emerge: (i) into the tropical stratosphere (tropical pipe), and (ii) into the Northern Hemisphere (NH) extratropical lower stratosphere. Maximum anticyclone air mass fractions reach around 5 % in the tropical pipe and 15 % in the extratropical lowermost stratosphere over the course of a year. The anticyclone air mass fraction correlates well with satellite hydrogen cyanide (HCN) and carbon monoxide (CO) observations, confirming that pollution is transported deep into the tropical stratosphere from the Asian monsoon anticyclone. Cross-tropopause transport occurs in a vertical chimney, but with the pollutants transported quasi-horizontally along isentropes above the tropopause into the tropics and NH.

Evidence of horizontal and vertical transport of water in the Southern Hemisphere tropical tropopause layer (TTL) from high-resolution balloon observations

Abstract. High-resolution in situ balloon measurements of water vapour, aerosol, methane and temperature in the upper tropical tropopause layer (TTL) and lower stratosphere are used to evaluate the processes affecting the stratospheric water budget: horizontal transport (in-mixing) and hydration by cross-tropopause overshooting updrafts. The obtained in situ evidence of these phenomena are analysed using satellite observations by Aura MLS (Microwave Limb Sounder) and CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) together with trajectory and transport modelling performed using CLaMS (Chemical Lagrangian Model of the Stratosphere) and HYSPLIT (Hybrid Single-Particle Lagrangian Integrated Trajectory) model. Balloon soundings were conducted during March 2012 in Bauru, Brazil (22.3° S) in the frame of the TRO-Pico campaign for studying the impact of convective overshooting on the stratospheric water budget. The balloon payloads included two stratospheric hygrometers: FLASH-B (Fluorescence Lyman-Alpha Stratospheric Hygrometer for Balloon) and Pico-SDLA instrument as well as COBALD (Compact Optical Backscatter Aerosol Detector) sondes, complemented by Vaisala RS92 radiosondes. Water vapour vertical profiles obtained independently by the two stratospheric hygrometers are in excellent agreement, ensuring credibility of the vertical structures observed. A signature of in-mixing is inferred from a series of vertical profiles, showing coincident enhancements in water vapour (of up to 0.5 ppmv) and aerosol at the 425 K (18.5 km) level. Trajectory analysis unambiguously links these features to intrusions from the Southern Hemisphere extratropical stratosphere, containing more water and aerosol, as demonstrated by MLS and CALIPSO global observations. The in-mixing is successfully reproduced by CLaMS simulations, showing a relatively moist filament extending to 20° S. A signature of local cross-tropopause transport of water is observed in a particular sounding, performed on a convective day and revealing water vapour enhancements of up to 0.6 ppmv as high as the 404 K (17.8 km) level. These are shown to originate from convective overshoots upwind detected by an S-band weather radar operating locally in Bauru. The accurate in situ observations uncover two independent moisture pathways into the tropical lower stratosphere, which are hardly detectable by space-borne sounders. We argue that the moistening by horizontal transport is limited by the weak meridional gradients of water, whereas the fast convective cross-tropopause transport, largely missed by global models, can have a substantial effect, at least at a regional scale.

A Probabilistic Multispectral Pattern Recognition Method for Detection of Overshooting Cloud Tops Using Passive Satellite Imager Observations

AbstractDeep convective updrafts often penetrate through the surrounding cirrus anvil and into the lower stratosphere. Cross-tropopause transport of ice, water vapor, and chemicals occurs within these “overshooting tops” (OTs) along with a variety of hazardous weather conditions. OTs are readily apparent in satellite imagery, and, given the importance of OTs for weather and climate, a number of automated satellite-based detection methods have been developed. Some of these methods have proven to be relatively reliable, and their products are used in diverse Earth science applications. Nevertheless, analysis of these methods and feedback from product users indicate that use of fixed infrared temperature–based detection criteria often induces biases that can limit their utility for weather and climate analysis. This paper describes a new multispectral OT detection approach that improves upon those previously developed by minimizing use of fixed criteria and incorporating pattern recognition analyses to arrive at an OT probability product. The product is developed and validated using OT and non-OT anvil regions identified by a human within MODIS imagery. The product offered high skill for discriminating between OTs and anvils and matched 69% of human OT identifications for a particular probability threshold with a false-detection rate of 18%, outperforming previously existing methods. The false-detection rate drops to 1% when OT-induced texture detected within visible imagery is used to constrain the IR-based OT probability product. The OT probability product is also shown to improve severe-storm detection over the United States by 20% relative to the best existing method.

Using beryllium-7 to assess cross-tropopause transport in global models

Abstract. We use the Global Modeling Initiative (GMI) modeling framework to assess the utility of cosmogenic beryllium-7 (7Be), a natural aerosol tracer, for evaluating cross-tropopause transport in global models. The GMI chemical transport model (CTM) was used to simulate atmospheric 7Be distributions using four different meteorological data sets (GEOS1-STRAT DAS, GISS II′ GCM, fvGCM, and GEOS4-DAS), featuring significantly different stratosphere–troposphere exchange (STE) characteristics. The simulations were compared with the upper troposphere and/or lower stratosphere (UT/LS) 7Be climatology constructed from ∼ 25 years of aircraft and balloon data, as well as climatological records of surface concentrations and deposition fluxes. Comparison of the fraction of surface air of stratospheric origin estimated from the 7Be simulations with observationally derived estimates indicates excessive cross-tropopause transport at mid-latitudes in simulations using GEOS1-STRAT and at high latitudes using GISS II′ meteorological data. These simulations also overestimate 7Be deposition fluxes at mid-latitudes (GEOS1-STRAT) and at high latitudes (GISS II′), respectively. We show that excessive cross-tropopause transport of 7Be corresponds to overestimated stratospheric contribution to tropospheric ozone. Our perspectives on STE in these meteorological fields based on 7Be simulations are consistent with previous modeling studies of tropospheric ozone using the same meteorological fields. We conclude that the observational constraints for 7Be and observed 7Be total deposition fluxes can be used routinely as a first-order assessment of cross-tropopause transport in global models.

Global-scale atmosphere monitoring by in-service aircraft – current achievements and future prospects of the European Research Infrastructure IAGOS

The European Research Infrastructure IAGOS (In-service Aircraft for a Global Observing System) operates a global-scale monitoring system for atmospheric trace gases, aerosols and clouds utilising the existing global civil aircraft. This new monitoring infrastructure builds on the heritage of the former research projects MOZAIC (Measurement of Ozone and Water Vapour on Airbus In-service Aircraft) and CARIBIC (Civil Aircraft for the Regular Investigation of the Atmosphere Based on an Instrument Container). CARIBIC continues within IAGOS and acts as an important airborne measurement reference standard within the wider IAGOS fleet. IAGOS is a major contributor to the in-situ component of the Copernicus Atmosphere Monitoring Service (CAMS), the successor to the Global Monitoring for the Environment and Security – Atmospheric Service, and is providing data for users in science, weather services and atmospherically relevant policy. IAGOS is unique in collecting regular in-situ observations of reactive gases, greenhouse gases and aerosol concentrations in the upper troposphere and lowermost stratosphere (UTLS) at high spatial resolution. It also provides routine vertical profiles of these species in the troposphere over continental sites or regions, many of which are undersampled by other networks or sampling studies, particularly in Africa, Southeast Asia and South America. In combination with MOZAIC and CARIBIC, IAGOS has provided long-term observations of atmospheric chemical composition in the UTLS since 1994. The longest time series are 20 yr of temperature, H2O and O3, and 9–15 yr of aerosols, CO, NOy, CO2, CH4, N2O, SF6, Hg, acetone, ~30 HFCs and ~20 non-methane hydrocarbons. Among the scientific highlights which have emerged from these data sets are observations of extreme concentrations of O3 and CO over the Pacific basin that have never or rarely been recorded over the Atlantic region for the past 12 yr; detailed information on the temporal and regional distributions of O3, CO, H2O, NOy and aerosol particles in the UTLS, including the impacts of cross-tropopause transport, deep convection and lightning on the distribution of these species; characterisation of ice-supersaturated regions in the UTLS; and finally, improved understanding of the spatial distribution of upper tropospheric humidity including the finding that the UTLS is much more humid than previously assumed.

Aerosol microphysics simulations of the Mt.~Pinatubo eruption with the UM-UKCA composition-climate model

Abstract. We use a stratosphere–troposphere composition–climate model with interactive sulfur chemistry and aerosol microphysics, to investigate the effect of the 1991 Mount Pinatubo eruption on stratospheric aerosol properties. Satellite measurements indicate that shortly after the eruption, between 14 and 23 Tg of SO2 (7 to 11.5 Tg of sulfur) was present in the tropical stratosphere. Best estimates of the peak global stratospheric aerosol burden are in the range 19 to 26 Tg, or 3.7 to 6.7 Tg of sulfur assuming a composition of between 59 and 77 % H2SO4. In light of this large uncertainty range, we performed two main simulations with 10 and 20 Tg of SO2 injected into the tropical lower stratosphere. Simulated stratospheric aerosol properties through the 1991 to 1995 period are compared against a range of available satellite and in situ measurements. Stratospheric aerosol optical depth (sAOD) and effective radius from both simulations show good qualitative agreement with the observations, with the timing of peak sAOD and decay timescale matching well with the observations in the tropics and mid-latitudes. However, injecting 20 Tg gives a factor of 2 too high stratospheric aerosol mass burden compared to the satellite data, with consequent strong high biases in simulated sAOD and surface area density, with the 10 Tg injection in much better agreement. Our model cannot explain the large fraction of the injected sulfur that the satellite-derived SO2 and aerosol burdens indicate was removed within the first few months after the eruption. We suggest that either there is an additional alternative loss pathway for the SO2 not included in our model (e.g. via accommodation into ash or ice in the volcanic cloud) or that a larger proportion of the injected sulfur was removed via cross-tropopause transport than in our simulations. We also critically evaluate the simulated evolution of the particle size distribution, comparing in detail to balloon-borne optical particle counter (OPC) measurements from Laramie, Wyoming, USA (41° N). Overall, the model captures remarkably well the complex variations in particle concentration profiles across the different OPC size channels. However, for the 19 to 27 km injection height-range used here, both runs have a modest high bias in the lowermost stratosphere for the finest particles (radii less than 250 nm), and the decay timescale is longer in the model for these particles, with a much later return to background conditions. Also, whereas the 10 Tg run compared best to the satellite measurements, a significant low bias is apparent in the coarser size channels in the volcanically perturbed lower stratosphere. Overall, our results suggest that, with appropriate calibration, aerosol microphysics models are capable of capturing the observed variation in particle size distribution in the stratosphere across both volcanically perturbed and quiescent conditions. Furthermore, additional sensitivity simulations suggest that predictions with the models are robust to uncertainties in sub-grid particle formation and nucleation rates in the stratosphere.

Tunable diode laser in-situ CH<sub>4</sub> measurements aboard the CARIBIC passenger aircraft: instrument performance assessment

Abstract. A laser spectrometer for automated monthly measurements of methane (CH4) mixing ratios aboard the CARIBIC passenger aircraft is presented. The instrument is based on a commercial Fast Greenhouse Gas Analyser (FGGA, Los Gatos Res.), which was adapted to meet the requirements imposed by unattended airborne operation. It was characterised in the laboratory with respect to instrument stability, precision, cross sensitivity to H2O, and accuracy. For airborne operation, a calibration strategy is described that utilises CH4 measurements obtained from flask samples taken during the same flights. The precision of airborne measurements is 2 ppb for 10 s averages. The accuracy at aircraft cruising altitude is 3.85 ppb. During aircraft ascent and descent, where no flask samples were obtained, instrumental drifts can be less accurately determined and the uncertainty is estimated to be 12.4 ppb. A linear humidity bias correction was applied to the CH4 measurements, which was most important in the lower troposphere. On average, the correction bias was around 6.5 ppb at an altitude of 2 km, and negligible at cruising flight level. Observations from 103 long-distance flights are presented that span a large part of the northern hemispheric upper troposphere and lowermost stratosphere (UT/LMS), with occasional crossing of the tropics on flights to southern Africa. These accurate data mark the largest UT/LMS in-situ CH4 dataset worldwide. An example of a tracer-tracer correlation study with ozone is given, highlighting the possibility for accurate cross-tropopause transport analyses.

Effects of sea surface temperature and greenhouse gas changes on the transport between the stratosphere and troposphere

[1] The effects of sea surface temperature (SST) and greenhouse gas (GHG) changes on the mean age-of-air and water vapor are investigated using a state-of-the-art general circulation model (GCM), and general characteristics of tracer transport between the stratosphere and troposphere are analyzed. Downward tracer transport in the northern midlatitude stratosphere is found to be faster than at southern midlatitudes. The global mean downward transport to the troposphere from stratosphere mainly occurs during northern winter and the downward cross-tropopause transport is weakest from August to October. The maximum troposphere mean (TM) age-of-air, derived from an age tracer released near the stratopause (around 1 hPa), can reach 13 years and is much larger than the maximum stratosphere mean (SM) age-of-air derived from an analogous age tracer released in the troposphere, with the SM age-of-air in the Northern Hemisphere being younger than in the Southern Hemisphere. Increased SSTs tend to accelerate upward transport through the stratosphere and slow downward transport in midlatitudes and the tropical stratosphere. In the context of effects of GHG increases and the associated SST increases on the stratosphere mean age-of-air, the GHG effects dominate, i.e., changes in the stratospheric mean age-of-air caused by SST increases only are smaller than those caused by combined changes in SSTs and GHGs. An increase in SSTs enhances the upward Eliasen-Palm (EP) flux in the extratropics. A 7.7% enhancement of tropical upwelling can be caused by a uniform 1.5 K SST increase. When both SST and GHG values are increased to the 2100 conditions, the meridional heat flux decreases in both winter hemispheres (and statistically significantly in the Southern Hemisphere). Meanwhile, the EP flux in the Northern Hemisphere increases significantly and the tropical upwelling is enhanced by 15% compared to the present-day conditions.

Cross Tropopause Transport of Water by Mid-Latitude Deep Convective Storms: A Review

Recent observational and numerical modeling studies of the mechanisms which transport moisture to the stratosphere by deep convective storms at mid-latitudes are reviewed. Observational evidence of the cross-tropopause transport of moisture by thunderstorms includes satellite, aircraft and ground-based data. The primary satellite evidence is taken from both conventional satellite of thunderstorm images and CloudSat vertical cloud cross-section images. The conventional satellite images show cirrus plumes above the anvil tops of some of the convective storms where the anvils are already at the tropopause level. The CloudSat image shows an indication of penetration of cirrus plume into the stratosphere. The aircraft observations consist of earlier observations of the ”jumping cirrus” phenomenon reported by Fujita and recent detection of ice particles in the stratospheric air associated with deep convective storms. The ground-based observations are video camera records of the jumping cirrus phenomenon occurring at the top of thunderstorm cells. Numerical model studies of the penetrative deep convective storms were performed utilizing a three-dimensional cloud dynamical model to simulate a typical severe storm which occurred in the US Midwest region on 2 August 1981. Model results indicate two physical mechanisms that cause water to be injected into the stratosphere from the storm: (1) the jumping cirrus mechanism which is caused by the gravity wave breaking at the cloud top, and (2) an instability caused by turbulent mixing in the outer shell of the overshooting dome. Implications of the penetrative convection on global processes and a brief future outlook are discussed.

Stratospheric water vapour budget and convection overshooting the tropopause: modelling study from SCOUT-AMMA

Abstract. The aim of this paper is to study the impacts of overshooting convection at a local scale on the water distribution in the tropical UTLS. Overshooting convection is assumed to be one of the processes controlling the entry of water vapour mixing ratio in the stratosphere by injecting ice crystals above the tropopause which later sublimate and hydrate the lower stratosphere. For this purpose, we quantify the individual impact of two cases of overshooting convection in Africa observed during SCOUT-AMMA: the case of 4 August 2006 over Southern Chad which is likely to have influenced the water vapour measurements by micro-SDLA and FLASH-B from Niamey on 5 August, and the case of a mesoscale convective system over Aïr on 5 August 2006. We make use of high resolution (down to 1 km horizontally) nested grid simulations with the three-dimensional regional atmospheric model BRAMS (Brazilian Regional Atmospheric Modelling System). In both cases, BRAMS succeeds in simulating the main features of the convective activity, as well as overshooting convection, though the exact position and time of the overshoots indicated by MSG brightness temperature difference is not fully reproduced (typically 1° displacement in latitude compared with the overshoots indicated by brightness temperature difference from satellite observations for both cases, and several hours shift for the Aïr case on 5 August 2006). Total water budgets associated with these two events show a significant injection of ice particles above the tropopause with maximum values of about 3.7 ton s−1 for the Chad case (4 August) and 1.4 ton s−1 for the Aïr case (5 August), and a total upward cross tropopause transport of about 3300 ton h−1 for the Chad case and 2400 ton h−1 for the Aïr case in the third domain of simulation. The order of magnitude of these modelled fluxes is lower but comparable with similar studies in other tropical areas based on models. These two estimations exhibit significant differences and highlight variability among the cases of the impact of overshooting convection in hydrating the lower stratosphere. We show that the regional enhancement of water above the tropopause is between 0.21 to 0.67 ppmv between 380 and 400 K, generally in the range of other model estimations. The amount of water which remains in the stratosphere after the overshoot is estimated for both cases. A range of 330 to 507 tons is found for the Chad case and an upper limit of 200 tons is found for the Aïr case. Finally we emphasize that the hydrated area in the LS by overshooting convection can be advected relatively far away from the overshoot initial location, with locally mixing ratios of more than 3 ppmv higher than the background level, which is compatible with the balloon borne measurements performed above Niamey in the same air mass, 30 h after the overshoot.

Further evidences of deep convective vertical transport of water vapor through the tropopause

A few years ago, we identified a deep convective transport mechanism, of water vapor through the tropopause, namely, storm top gravity wave breaking, such that tropospheric water substance can be injected into the lower stratosphere via this pathway. The main evidence presented previously was taken from the lower resolution AVHRR images of the storm anvil top cirrus plumes obtained by polar orbiting satellites. Recent observations have provided further supporting evidence for this important cross-tropopause transport mechanism. There are now many higher resolution satellite images, mainly from MODIS instrument, that show more definitely the existence of these plumes, many of which would probably be unseen by lower resolution images. Furthermore, a thunderstorm movie taken in Denver (USA) area during STEPS2000 field campaign and another thunderstorm movie taken by a building top webcam in Zurich also demonstrate that the jumping cirrus phenomenon, first identified by T. Fujita in 1980s, may be quite common in active thunderstorm cells, quite contrary to previous belief that it is rare. We have used a cloud model to demonstrate that the jumping cirrus is exactly the gravity wave breaking phenomenon that transports water vapor through the tropopause. These additional evidences provide increasing support that deep convection contributes substantially to the troposphere-to-stratosphere transport of water substance. This corroborates well with recent studies of the stratospheric HDO/H 2O ratio which is much highly than it would be if the transport is via slow ascent. The only explanation that can be used to interpret this observation at present is that water substance is transported through the tropopause via rapid vertical motion, i.e., deep convection.