Upper Troposphere And Lowermost Stratosphere Research Articles

Pollution trace gases C<sub>2</sub>H<sub>6</sub>, C<sub>2</sub>H<sub>2</sub>, HCOOH, and PAN in the North Atlantic UTLS: observations and simulations

Abstract. Measurements of the pollution trace gases ethane (C2H6), ethyne (C2H2), formic acid (HCOOH), and peroxyacetyl nitrate (PAN) were performed in the North Atlantic upper troposphere and lowermost stratosphere (UTLS) region with the airborne limb imager GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) with high spatial resolution down to cloud top. Observations were made during flights with the German research aircraft HALO (High Altitude and LOng Range Research Aircraft) in the frame of the WISE (Wave-driven ISentropic Exchange) campaign, which was carried out in autumn 2017 from Shannon (Ireland) and Oberpfaffenhofen (Germany). Enhanced volume mixing ratios (VMRs) of up to 2.2 ppbv C2H6, 0.2 ppbv C2H2, 0.9 ppbv HCOOH, and 0.4 ppbv PAN were detected during the flight on 13 September 2017 in the upper troposphere and around the tropopause above the British Isles. Elevated quantities of PAN were measured even in the lowermost stratosphere (locally up to 14 km), likely reflecting the fact that this molecule has the longest lifetime of the four species discussed herein. Backward trajectory calculations as well as global three-dimensional Chemical Lagrangian Model of the Stratosphere (CLaMS) simulations with artificial tracers of air mass origin have shown that the main sources of the observed pollutant species are forest fires in North America and anthropogenic pollution in South Asia and Southeast Asia uplifted and moved within the Asian monsoon anticyclone (AMA) circulation system. After release from the AMA, these species or their precursor substances are transported by strong tropospheric winds over large distances, depending on their particular atmospheric lifetime of up to months. Observations are compared to simulations with the atmospheric models EMAC (ECHAM5/MESSy Atmospheric Chemistry) and CAMS (Copernicus Atmosphere Monitoring Service). These models are qualitatively able to reproduce the measured VMR enhancements but underestimate the absolute amount of the increase. Increasing the emissions in EMAC by a factor of 2 reduces the disagreement between simulated and measured results and illustrates the importance of the quality of emission databases used in chemical models.

Pollution trace gas distributions and their transport in the Asian monsoon upper troposphere and lowermost stratosphere during the StratoClim campaign 2017

Abstract. We present the first high-resolution measurements of pollutant trace gases in the Asian summer monsoon upper troposphere and lowermost stratosphere (UTLS) from the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) during the StratoClim (Stratospheric and upper tropospheric processes for better climate predictions) campaign based in Kathmandu, Nepal, 2017. Measurements of peroxyacetyl nitrate (PAN), acetylene (C2H2), and formic acid (HCOOH) show strong local enhancements up to altitudes of 16 km. More than 500 pptv of PAN, more than 200 pptv of C2H2, and more than 200 pptv of HCOOH are observed. Air masses with increased volume mixing ratios of PAN and C2H2 at altitudes up to 18 km, reaching to the lowermost stratosphere, were present at these altitudes for more than 10 d, as indicated by trajectory analysis. A local minimum of HCOOH is correlated with a previously reported maximum of ammonia (NH3), which suggests different washout efficiencies of these species in the same air masses. A backward trajectory analysis based on the models Alfred Wegener InsTitute LAgrangian Chemistry/Transport System (ATLAS) and TRACZILLA, using advanced techniques for detection of convective events, and starting at geolocations of GLORIA measurements with enhanced pollution trace gas concentrations, has been performed. The analysis shows that convective events along trajectories leading to GLORIA measurements with enhanced pollutants are located close to regions where satellite measurements by the Ozone Monitoring Instrument (OMI) indicate enhanced tropospheric columns of nitrogen dioxide (NO2) in the days prior to the observation. A comparison to the global atmospheric models Copernicus Atmosphere Monitoring Service (CAMS) and ECHAM/MESSy Atmospheric Chemistry (EMAC) has been performed. It is shown that these models are able to reproduce large-scale structures of the pollution trace gas distributions for one part of the flight, while the other part of the flight reveals large discrepancies between models and measurement. These discrepancies possibly result from convective events that are not resolved or parameterized in the models, uncertainties in the emissions of source gases, and uncertainties in the rate constants of chemical reactions.

An emission module for ICON-ART 2.0: implementation and simulations of acetone

Abstract. We present a recently developed emission module for the ICON (ICOsahedral Non-hydrostatic)-ART (Aerosols and Reactive Trace gases) modelling framework. The emission module processes external flux data sets and increments the tracer volume mixing ratios in the boundary layer accordingly. The performance of the emission module is illustrated with simulations of acetone, using a simplified chemical depletion mechanism based on a reaction with OH and photolysis only. In our model setup, we calculate a tropospheric acetone lifetime of 33 days, which is in good agreement with the literature. We compare our results with ground-based as well as with airborne IAGOS-CARIBIC measurements in the upper troposphere and lowermost stratosphere (UTLS) in terms of phase and amplitude of the annual cycle. In all our ICON-ART simulations the general seasonal variability is well represented but uncertainties remain concerning the magnitude of the acetone mixing ratio in the UTLS region. In addition, the module for online calculations of biogenic emissions (MEGAN2.1) is implemented in ICON-ART and can replace the offline biogenic emission data sets. In a sensitivity study we show how different parametrisations of the leaf area index (LAI) change the emission fluxes calculated by MEGAN2.1 and demonstrate the importance of an adequate treatment of the LAI within MEGAN2.1. We conclude that the emission module performs well with offline and online emission fluxes and allows the simulation of the annual cycles of emissions-dominated substances.

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.

Technical Note: Reanalysis of upper troposphere humidity data from the MOZAIC programme for the period 1994 to 2009

Abstract. In situ observational data on the relative humidity (RH) in the upper troposphere and lowermost stratosphere (UT/LS), or tropopause region, collected aboard civil passenger aircraft in the MOZAIC (Measurements of OZone, water vapour, carbon monoxide and nitrogen oxides by in-service AIrbus airCraft) programme were reanalysed for the period 2000 to 2009. Previous analyses of probability distribution functions (PDFs) of upper troposphere humidity (UTH) data from MOZAIC observations from year 2000 and later indicated a bias of UTH data towards higher RH values compared to data of the period 1994 to 1999. As a result, the PDF of UTH data show a substantial fraction of observations above 100% relative humidity with respect to liquid water. Such supersaturations, however, do not occur in the atmosphere because there is always a sufficient number of condensation nuclei available, that trigger condensation as soon as liquid saturation is slightly exceeded. An in-depth reanalysis of the data set identified a coding error in the calibration procedure from year 2000 on. The error did not affect earlier data from 1994 to 1999. The full data set for 2000–2009 was reanalysed applying the corrected calibration procedure. Applied correction schemes and a revised error analysis are presented along with the reanalysed PDF of relative humidity with respect to liquid water (RHliquid) and ice (RHice).

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.

Sub‐micrometer aerosol particles in the upper troposphere/lowermost stratosphere as measured by CARIBIC and modeled using the MIT‐CAM3 global climate model

In this study, we compare modeled (MIT‐CAM3) and observed (CARIBIC) sub‐micrometer nucleation (N4–12, 4 ≤ d ≤ 12 nm) and Aitken mode (N12, d > 12 nm) particle number concentrations in the upper troposphere and lowermost stratosphere (UT/LMS). Modeled and observed global median N4–12 and N12 agree fairly well (within a factor of two) indicating that the relatively simplified binary H2SO4‐H2O nucleation parameterization applied in the model produces reasonable results in the UT/LMS. However, a comparison of the spatiotemporal distribution of sub‐micrometer particles displays a number of discrepancies between MIT‐CAM3 and CARIBIC data: N4–12is underestimated by the model in the tropics and overestimated in the extra‐topics. N12 is in general overestimated by the model, in particular in the tropics and during summer months. The modeled seasonal variability of N4–12 is in poor agreement with CARIBIC data whereas it agrees rather well for N12. Modeled particle frequency distributions are in general narrower than the observed ones. The model biases indicate an insufficient diffusive mixing in MIT‐CAM3 and a too large vertical transport of carbonaceous aerosols. The overestimated transport is most likely caused by the constant supersaturation threshold applied in the model for the activation of particles into cloud droplets. The annually constant SO2 emissions in the model may also partly explain the poor representation of the N4–12seasonal cycle. Comparing the MIT‐CAM3 with CARIBIC data, it is also clear that care has to be taken regarding the representativeness of the measurement data and the time frequency of the model output.

Near-global aerosol mapping in the upper troposphere and lowermost stratosphere with data from the CARIBIC project

This study extrapolates aerosol data of the CARIBIC project from 1997 until June 2008 in along trajectories to compose large-scale maps and vertical profiles of submicrometre particle concentrations in the upper troposphere and lowermost stratosphere (UT/LMS). The extrapolation was validated by comparing extrapolated values with CARIBIC data measured near the respective trajectory position and by comparing extrapolated CARIBIC data to measurements by other experiments near the respective trajectory positions. Best agreement between extrapolated and measured data is achieved with particle lifetimes longer than the maximum length of used trajectories. The derived maps reveal regions of strong and frequent new particle formation, namely the Tropical Central and Western Africa with the adjacent Atlantic, South America, the Caribbean and Southeast Asia. These regions of particle formation coincide with those of frequent deep convective clouds. Vertical particle concentration profiles for the troposphere and the stratosphere confirm statistically previous results indicating frequent new particle formation in the tropopause region. There was no statistically significant increase in Aitken mode particle concentration between the first period of CARIBIC operation, 1997–2002, and the second period, 2004–2009. However, a significant increase in concentration occurred within the latter period when considering it in isolation.

Variability of active chlorine in the lowermost Arctic stratosphere

We examine the variability of ClO in the Arctic upper troposphere and lowermost stratosphere (UTLS) during the winter of 1999–2000. Data are binned relative to NOy, a species that is a proxy for photochemical age and a photochemical source of NOx. Enhancements in the [ClO]/[Cly] ratio relative to values expected from gas‐phase chemistry alone were observed throughout the region and were largest in the coldest sampled regions, where T < 208 K. At low NOy values, where particles containing NOy and water were often detected, twilight ClO abundances in the afternoon were nearly a factor of 3 larger than those in the morning. At higher NOy values, where much lower particle surface areas were measured, ClO abundances in morning twilight were somewhat larger than those in the afternoon. These observations are consistent with a daytime mechanism of rapid heterogeneous activation of inorganic chlorine in particle‐rich, low‐NOy regions, with slower deactivation in relatively particle‐poor, higher‐NOy regions of the lowermost stratosphere. While the data clearly show widespread chlorine activation, knowledge of the precise value of the [ClO]/[Cly] ratio is limited because of the lack of available data on inorganic chlorine species, notably HCl, believed to be the dominant reservoir of inorganic chlorine at these altitudes.

Simulating the global atmospheric black carbon cycle: a revisit to the contribution of aircraft emissions

Abstract. The black carbon (BC) burden of the upper troposphere and lowermost stratosphere (UTLS) is investigated with the general circulation model (GCM) ECHAM4. The special focus is the contribution of aircraft emissions to the UTLS BC loading. Previous studies on the role of aircraft emissions in the global BC cycle either neglect BC sources located at the Earth's surface or simplify the BC cycle by assuming pre-defined BC residence times. Here, the global BC cycle including emissions, transport, and removal is explicitly simulated. The BC emissions considered include surface sources as well as BC from aviation. This enables a consistent calculation of the relative contribution of aviation to the global atmospheric BC cycle. As a further extension to the previous studies, the aviation-induced perturbation of the UTLS BC particle number concentration is investigated. The uncertainties associated with the model predictions are evaluated by means of several sensitivity studies. Especially, the sensitivity of the results to different assumptions on the BC hygroscopic properties is analysed. The simulated UTLS BC concentrations are compared to in-situ observations. The simulations suggest that the large-scale contribution of aviation to the UTLS BC mass budget typically amounts to only a few percent, even in the most frequented flight regions. The aviation impact far away from these regions is negligible. The simulated aircraft contributions to the UTLS BC particle number concentration are much larger compared to the corresponding mass perturbations. The simulations suggest that aviation can cause large-scale increases in the UTLS BC particle number concentration of more than 30% in regions highly frequented by aircraft. The relative effect shows a pronounced annual variation with the largest relative aviation impact occurring during winter.