Chemical Lagrangian Model Of The Stratosphere Research Articles

A multi-scenario Lagrangian trajectory analysis to identify source regions of the Asian tropopause aerosol layer on the Indian subcontinent in August 2016

Abstract. The Asian tropopause aerosol layer (ATAL) is present during the Asian summer monsoon season affecting the radiative balance of the atmosphere. However, the source regions and transport pathways of ATAL particles are still uncertain. Here, we investigate transport pathways from different regions at the model boundary layer (MBL) to the ATAL by combining two Lagrangian transport models (CLaMS, Chemical Lagrangian Model of the Stratosphere; MPTRAC, Massive-Parallel Trajectory Calculations) with balloon-borne measurements of the ATAL performed by the Compact Optical Backscatter Aerosol Detector (COBALD) above Nainital (India) in August 2016. Trajectories are initialised at the measured location of the ATAL and calculated 90 d backwards in time to investigate the relation between the measured, daily averaged, aerosol backscatter ratio and source regions at the MBL. Different simulation scenarios are performed to find differences and robust patterns when the reanalysis data (ERA5 or ERA-Interim), the trajectory model, the vertical coordinate (kinematic and diabatic approach) or the convective parameterisation are varied. The robust finding among all scenarios is that the largest continental air mass contributions originate from the Tibetan Plateau and the Indian subcontinent (mostly the Indo-Gangetic Plain), and the largest maritime air mass contributions in Asia come from the western Pacific (e.g. related to tropical cyclones). Additionally, all simulation scenarios indicate that the transport of maritime air from the tropical western Pacific to the region of the ATAL lowers the backscatter ratio (BSR) of the ATAL, while most scenarios indicate that the transport of polluted air from the Indo-Gangetic Plain increases the BSR. While the results corroborate key findings from previous ERA-Interim-based studies, they also highlight the variability in the contributions of different MBL regions to the ATAL depending on different simulation scenarios.

Evaluation of vertical transport in ERA5 and ERA-Interim reanalysis using high-altitude aircraft measurements in the Asian summer monsoon 2017

Abstract. During the Asian monsoon season, greenhouse gases and pollution emitted near the ground are rapidly uplifted by convection up to an altitude of ∼ 13 km, with slower ascent and mixing with the stratospheric background above. Here, we address the robustness of the representation of these transport processes in different reanalysis data sets using ERA5, ERA-Interim and ERA5 1∘×1∘. This transport assessment includes the mean age of air from global three-dimensional simulations by the Lagrangian transport model CLaMS (Chemical Lagrangian Model of the Stratosphere), as well as different trajectory-based transport times and associated ascent rates compared with observation-based age of air and ascent rates of long-lived trace gases from airborne measurements during the Asian summer monsoon 2017 in Nepal. Our findings confirm that the ERA5 reanalysis yields a better representation of convection than ERA-Interim, resulting in different transport times and air mass origins at the Earth's surface. In the Asian monsoon region above 430 K, the mean age of air driven by ERA-Interim is too young, whereas the mean age of air from ERA5 1∘×1∘ is too old but somewhat closer to the observations. The mean effective ascent rates derived from ERA5 and ERA5 1∘×1∘ back trajectories are in good agreement with the observation-based mean ascent rates, unlike ERA-Interim, which is much faster above 430 K. Although a reliable CO2 reconstruction is a challenge for model simulations, we show that, up to 410 K, the CO2 reconstruction using ERA5 agrees best with high-resolution in situ aircraft CO2 measurements, indicating a better representation of Asian monsoon transport in the newest ECMWF reanalysis product, ERA5.

The Mission Support System (MSS v7.0.4) and its use in planning for the SouthTRAC aircraft campaign

Abstract. The Mission Support System (MSS) is an open source software package that has been used for planning flight tracks of scientific aircraft in multiple measurement campaigns during the last decade. It consists of three major components: a web map server located close to the model data storage site that is capable of producing a variety of 2-D figures from 4-D meteorological data; a client application capable of displaying the figures in combination with the planned flight track and an assortment of additional information; and a new collaboration server component that enables real-time collaboration of multiple remote parties. During the last decade, these components were constantly improved towards being simple to set up and use and being standard compliant. Here, we describe the use of MSS during the Southern Hemisphere Transport, Dynamics, and Chemistry–Gravity Waves (SouthTRAC-GW) measurement campaign in 2019. This campaign, based in Rio Grande, Argentina, used the German research aircraft HALO to investigate several scientific objectives related to the Southern Hemisphere chemistry and dynamics. We present the diverse data products offered by the MSS web map server dedicated to the campaign, which were derived from the European Centre for Medium-Range Weather Forecasts (ECMWF) forecast data, Chemical Lagrangian Model of the Stratosphere (CLaMS) simulations, and Atmospheric Infrared Sounder (AIRS) near-real time brightness temperature measurements. As an example for how the MSS software is used in conjunction with the different data sets, we describe the planning of a single flight, which eventually took place on 12 September 2019, probing orographic gravity waves propagating up into the lower mesosphere.

Tropospheric transport and unresolved convection: numerical experiments with CLaMS 2.0/MESSy

Abstract. Pure Lagrangian, i.e., trajectory-based transport models, take into account only the resolved advective part of transport. That means neither mixing processes between the air parcels (APs) nor unresolved subgrid-scale advective processes like convection are included. The Chemical Lagrangian Model of the Stratosphere (CLaMS 1.0) extends this approach by including mixing between the Lagrangian APs parameterizing the small-scale isentropic mixing. To improve model representation of the upper troposphere and lower stratosphere (UTLS), this approach was extended by taking into account parameterization of tropospheric mixing and unresolved convection in the recently published CLaMS 2.0 version. All three transport modes, i.e., isentropic and tropospheric mixing and the unresolved convection can be adjusted and optimized within the model. Here, we investigate the sensitivity of the model representation of tracers in the UTLS with respect to these three modes. For this reason, the CLaMS 2.0 version implemented within the Modular Earth Submodel System (MESSy), CLaMS 2.0/MESSy, is applied with meteorology based on the ERA-Interim (EI) and ERA5 (E5) reanalyses with the same horizontal resolution (1.0×1.0∘) but with 60 and 137 model levels for EI and E5, respectively. Comparisons with in situ observations are used to rate the degree of agreement between different model configurations and observations. Starting from pure advective runs as a reference and in agreement with CLaMS 1.0, we show that among the three processes considered, isentropic mixing dominates transport in the UTLS. Both the observed CO, O3, N2O, and CO2 profiles and CO–O3 correlations are clearly better reproduced in the model with isentropic mixing. The second most important transport process considered is convection which is only partially resolved in the vertical velocity fields provided by the analysis. This additional pathway of transport from the planetary boundary layer (PBL) to the main convective outflow dominates the composition of air in the lower stratosphere relative to the contribution of the resolved transport. This transport happens mainly in the tropics and sub-tropics, and significantly rejuvenates the age of air in this region. By taking into account tropospheric mixing, weakest changes in tracer distributions without any clear improvements were found.

How can Brewer–Dobson circulation trends be estimated from changes in stratospheric water vapour and methane?

Abstract. The stratospheric meridional overturning circulation, also referred to as the Brewer–Dobson circulation (BDC), controls the composition of the stratosphere, which, in turn, affects radiation and climate. As the BDC cannot be directly measured, one has to infer its strength and trends indirectly. For instance, trace gas measurements allow the calculation of average transit times. Satellite measurements provide information on the distributions of trace gases for the entire stratosphere, with measurements of particularly long temporal and dense spatial coverage available for stratospheric water vapour (H2O). Although chemical processes and boundary conditions confound interpretation, the influence of methane (CH4) oxidation on H2O in the stratosphere is relatively straightforward, and thus H2O is an appealing tracer for transport analysis despite these caveats. In this work, we explore how mean age of air trends can be estimated from the combination of stratospheric H2O and CH4 data, by carrying out a proof of concept within the model environment of the Chemical Lagrangian Model of the Stratosphere (CLaMS). In particular, we assess the methodological uncertainties related to the two commonly used approximations of (i) instantaneous stratospheric entry mixing ratio propagation and (ii) constant correlation between mean age and the fractional release factor of CH4. Performing various sensitivity studies with CLaMS, we test different methods of the mean age of air trend estimation, and we aim to provide simple and practical advice on the adjustment of the used approximations for obtaining more reliable mean age of air trends from the measurements of H2O and CH4. Our results show that the estimated mean age of air trends from the combination of stratospheric H2O and CH4 changes may be significantly affected by the assumed approximations. Depending on the investigated stratospheric region and the considered period, the error in estimated mean age of air trends can be large, especially in the lower stratosphere. For particular periods, the errors from the two approximations can lead to opposite effects, which may even cancel out. Finally, for a more reliable estimate of the mean age of air trends, we propose adjusting the approximation method by using an idealized age spectrum to propagate stratospheric entry mixing ratios. The findings of this work can be used for assessing the uncertainties in stratospheric BDC trend estimation from global satellite measurements.

Hemispheric asymmetries in recent changes in the stratospheric circulation

Abstract. The expected effect of ozone recovery on the stratospheric Brewer–Dobson circulation (BDC) is a slow-down, strongest in the Southern Hemisphere (SH). In contrast, the BDC has been found to weaken more strongly in the Northern Hemisphere (NH) relative to the SH in recent decades, inducing substantial effects on chemical composition. We investigate hemispheric asymmetries in BDC changes since about 2000 in simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS) driven with different reanalyses (ERA5, ERA-Interim, JRA-55, MERRA-2) and contrast those to free-running climate model simulations. We find that age-of-air increases robustly in the NH stratosphere relative to the SH in all reanalyses. Related nitrous oxide changes agree well between reanalysis-driven simulations and satellite measurements, providing observational evidence for the hemispheric asymmetry in BDC changes. We show that the composition changes in reanalyses are caused by structural residual-circulation changes related to an upward shift and strengthening of the deep BDC branch, resulting in longer transit times, and a downward shift and weakening shallow branch in the NH relative to the SH. Although climate model simulations show that ozone recovery will lead to overall reduced circulation and age-of-air trends, the hemispherically asymmetric signal in circulation trends is small compared to internal variability. Therefore, observed circulation trends over the recent past are not in contradiction to expectations from climate models. Furthermore, the hemispheric asymmetry in BDC trends imprints on the composition of the lower stratosphere, and the signal might propagate into the troposphere, potentially affecting composition down to the surface.

Characterization of transport from the Asian summer monsoon anticyclone into the UTLS via shedding of low potential vorticity cutoffs

Abstract. Air mass transport within the summertime Asian monsoon circulation provides a major source of anthropogenic pollution for the upper troposphere and lower stratosphere (UTLS). Here, we investigate the quasi-horizontal transport of air masses from the Asian summer monsoon anticyclone (ASMA) into the extratropical lower stratosphere and their chemical evolution. For that reason, we developed a method to identify and track the air masses exported from the monsoon. This method is based on the anomalously low potential vorticity (PV) of these air masses (tropospheric low PV cutoffs) compared to the lower stratosphere and uses trajectory calculations and chemical fields from the Chemical Lagrangian Model of the Stratosphere (CLaMS). The results show evidence of frequent summertime transport from the monsoon anticyclone to midlatitudes over the North Pacific, even reaching the high-latitude regions of Siberia and Alaska. Most of the low PV cutoffs related to air masses exported from the ASMA have lifetimes shorter than 1 week (about 90 %) and sizes smaller than 1 % of the Northern Hemisphere (NH) area. The chemical composition of these air masses is characterized by carbon monoxide, ozone, and water vapour mixing ratios at an intermediate range between values typical for the monsoon anticyclone and the lower stratosphere. The chemical evolution during transport within these low PV cutoffs shows a gradual change from the characteristics of the monsoon anticyclone to characteristics of the lower stratospheric background during about 1 week, indicating continuous mixing with the background atmosphere.

Simulation of Record Arctic Stratospheric Ozone Depletion in 2020

AbstractIn the Arctic winter/spring of 2019/2020, stratospheric temperatures were exceptionally low until early April and the polar vortex was very stable. As a consequence, significant chemical ozone depletion occurred in the Arctic polar vortex in spring 2020. Here, we present simulations using the Chemical Lagrangian Model of the Stratosphere that address the development of chlorine compounds and ozone in the Arctic stratosphere in 2020. The simulation reproduces relevant observations of ozone and chlorine compounds, as shown by comparisons with data from the Microwave Limb Sounder, Atmospheric Chemistry Experiment‐Fourier Transform Spectrometer, balloon‐borne ozone sondes, and the Ozone Monitoring Instrument. Although the concentration of chlorine and bromine compounds in the polar stratosphere has decreased by more than 10% compared to peak values around the year 2000, the meteorological conditions in winter/spring 2019/2020 caused unprecedented ozone depletion. The lowest simulated ozone mixing ratio was about 40 ppbv. Because extremely low ozone mixing ratios were reached in the lower polar stratosphere, chlorine deactivation into HCl occurred as is normally observed in the Antarctic polar vortex. The depletion in partial column ozone in the lower stratosphere (potential temperature from 350 to 600 K, corresponding to about 12–24 km) in the vortex core was calculated to reach 143 Dobson Units, which is more than the ozone loss in 2011 and 2016, the years which —until 2020— had seen the largest Arctic ozone depletion on record.

The stratospheric Brewer–Dobson circulation inferred from age of air in the ERA5 reanalysis

Abstract. This paper investigates the global stratospheric Brewer–Dobson circulation (BDC) in the ERA5 meteorological reanalysis from the European Centre for Medium-Range Weather Forecasts (ECMWF). The analysis is based on simulations of stratospheric mean age of air, including the full age spectrum, with the Lagrangian transport model CLaMS (Chemical Lagrangian Model of the Stratosphere), driven by reanalysis winds and total diabatic heating rates. ERA5-based results are compared to results based on the preceding ERA-Interim reanalysis. Our results show a significantly slower BDC for ERA5 than for ERA-Interim, manifesting in weaker diabatic heating rates and higher age of air. In the tropical lower stratosphere, heating rates are 30 %–40 % weaker in ERA5, likely correcting a bias in ERA-Interim. At 20 km and in the Northern Hemisphere (NH) stratosphere, ERA5 age values are around the upper margin of the uncertainty range from historical tracer observations, indicating a somewhat slow–biased BDC. The age trend in ERA5 over the 1989–2018 period is negative throughout the stratosphere, as climate models predict in response to global warming. However, the age decrease is not linear but steplike, potentially caused by multi-annual variability or changes in the observations included in the assimilation. During the 2002–2012 period, the ERA5 age shows a similar hemispheric dipole trend pattern as ERA-Interim, with age increasing in the NH and decreasing in the Southern Hemisphere (SH). Shifts in the age spectrum peak and residual circulation transit times indicate that reanalysis differences in age are likely caused by differences in the residual circulation. In particular, the shallow BDC branch accelerates in both reanalyses, whereas the deep branch accelerates in ERA5 and decelerates in ERA-Interim.

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.

Deep stratospheric intrusion and Russian wildfire induce enhanced tropospheric ozone pollution over the northern Tibetan Plateau

By using ozonesonde measurements during July–August in 2016, 2019, and 2020 at Golmud and Qaidam, European Centre for Medium-Range Weather Forecasts (ECMWF) next-generation reanalysis ERA5 data, satellite-borne Moderate Resolution Imaging Spectrometer data products, and backward trajectory calculations from the chemical Lagrangian model of the stratosphere (CLaMS) model, this study analyzes vertical ozone distributions and explores the influence of deep stratospheric intrusions and wildfires on ozone variation in the northern Tibetan Plateau (TP) during the Asian summer monsoon period. Large ozone partial pressures were observed between 20 and 30 km, with a maximum of ~16 mPa at approximately 27 km latitude. The comparisons between the vertical ozone profiles with and without the occurrence of stratospheric intrusions showed that their relative ozone difference was up to 72.4% in the tropopause layer (15.8 km), and a secondary maximum of 66.7% existed in the middle troposphere (10.1 km). The stratospheric intrusions dried the atmosphere by 52.9% and enhanced the ozone columns by 26.1% below the upper troposphere and lower stratosphere. A case study of deep stratospheric intrusion exhibited the occurrence of large ozone partial pressure in the middle troposphere in detail, with an ozone peak of ~6 mPa at 10 km, which was caused by a tropopause fold associated with the westerly wind jet at the north flank of the Asian summer monsoon anticyclone. The stratospheric intrusion processes effectively transported the cold and dry air mass with high ozone in the stratosphere downward to the middle troposphere over the northern TP. This study also confirmed that by long-range transport processes, large wildfire smoke occurred around central and eastern Russia on 19–26 July 2016 greatly caused ozone pollution in the troposphere (6 km depth from the surface) over the northern TP.

Asymmetry and pathways of inter-hemispheric transport in the upper troposphere and lower stratosphere

Abstract. Inter-hemispheric transport may strongly affect the trace gas composition of the atmosphere, especially in relation to anthropogenic emissions, which originate mainly in the Northern Hemisphere. This study investigates the transport from the boundary surface layer of the northern hemispheric (NH) extratropics (30–90∘ N), southern hemispheric (SH) extratropics (30–90∘ S), and tropics (30∘ S–30∘ N) into the global upper troposphere and lower stratosphere (UTLS) using simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS). In particular, we diagnose inter-hemispheric transport in terms of the air mass fractions (AMFs), age spectra, and the mean age of air (AoA) calculated for these three source regions. We find that the AMFs from the NH extratropics to the UTLS are about 5 times larger than the corresponding contributions from the SH extratropics and almost 20 times smaller than those from the tropics. The amplitude of the AMF seasonal variability originating from the NH extratropics is comparable to that from the tropics. The NH and SH extratropical age spectra show much stronger seasonality compared to the seasonality of the tropical age spectra. The transit time of NH-extratropical-origin air to the SH extratropics is longer than vice versa. The asymmetry of the inter-hemispheric transport is mainly driven by the Asian summer monsoon (ASM). We confirm the important role of ASM and westerly ducts in the inter-hemispheric transport from the NH extratropics to the SH. Furthermore, we find that it is an interplay between the ASM and westerly ducts which triggers such cross-Equator transport from boreal summer to fall in the UTLS between 350 and 370 K.

Potential of future stratospheric ozone loss in the midlatitudes under global warming and sulfate geoengineering

Abstract. The potential of heterogeneous chlorine activation in the midlatitude lowermost stratosphere during summer is a matter of debate. The occurrence of heterogeneous chlorine activation through the presence of aerosol particles could cause ozone destruction. This chemical process requires low temperatures and is accelerated by an enhancement of the stratospheric water vapour and sulfate amount. In particular, the conditions present in the lowermost stratosphere during the North American Summer Monsoon season (NAM) are expected to be cold and moist enough to cause the occurrence of heterogeneous chlorine activation. Furthermore, the temperatures, the water vapour mixing ratio and the sulfate aerosol abundance are affected by future global warming and by the potential application of sulfate geoengineering. Hence, both future scenarios could promote this ozone destruction process. We investigate the likelihood of the occurrence of heterogeneous chlorine activation and its impact on ozone in the lowermost-stratospheric mixing layer between tropospheric and stratospheric air above central North America (30.6–49.6∘ N, 72.25–124.75∘ W) in summer for conditions today, at the middle and at the end of the 21st century. Therefore, the results of the Geoengineering Large Ensemble Simulations (GLENS) for the lowermost-stratospheric mixing layer between tropospheric and stratospheric air are considered together with 10-day box-model simulations performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS). In GLENS two future scenarios are simulated: the RCP8.5 global warming scenario and a geoengineering scenario, where sulfur is additionally injected into the stratosphere to keep the global mean surface temperature from changing. In the GLENS simulations, the mixing layer will warm and moisten in both future scenarios with a larger effect in the geoengineering scenario. The likelihood of chlorine activation occurring in the mixing layer is highest in the years 2040–2050 if geoengineering is applied, accounting for 3.3 %. In comparison, the likelihood of conditions today is 1.0 %. At the end of the 21st century, the likelihood of this ozone destruction process occurring decreases. We found that 0.1 % of the ozone mixing ratios in the mixing layer above central North America is destroyed for conditions today. A maximum ozone destruction of 0.3 % in the mixing layer occurs in the years 2040–2050 if geoengineering is applied. Comparing the southernmost latitude band (30–35∘ N) and the northernmost latitude band (44–49∘ N) of the considered region, we found a higher likelihood of the occurrence of heterogeneous chlorine activation in the southernmost latitude band, causing a higher impact on ozone as well. However, the ozone loss process is found to have a minor impact on the midlatitude ozone column.

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.

Strong day-to-day variability of the Asian Tropopause Aerosol Layer (ATAL) in August 2016 at the Himalayan foothills

Abstract. The South Asian summer monsoon is associated with a large-scale anticyclonic circulation in the upper troposphere and lower stratosphere (UTLS), which confines the air mass inside. During boreal summer, the confinement of this air mass leads to an accumulation of aerosol between about 13 and 18 km (360 and 440 K potential temperature); this accumulation of aerosol constitutes the Asian Tropopause Aerosol Layer (ATAL). We present balloon-borne aerosol backscatter measurements of the ATAL performed by the Compact Optical Backscatter Aerosol Detector (COBALD) instrument in Nainital in northern India in August 2016, and compare these with COBALD measurements in the post-monsoon time in November 2016. The measurements demonstrate a strong variability of the ATAL's altitude, vertical extent, aerosol backscatter intensity and cirrus cloud occurrence frequency. Such a variability cannot be deduced from climatological means of the ATAL as they are derived from satellite measurements. To explain this observed variability we performed a Lagrangian back-trajectory analysis using the Chemical Lagrangian Model of the Stratosphere (CLaMS). We identify the transport pathways as well as the source regions of air parcels contributing to the ATAL over Nainital in August 2016. Our analysis reveals a variety of factors contributing to the observed day-to-day variability of the ATAL: continental convection, tropical cyclones (maritime convection), dynamics of the anticyclone and stratospheric intrusions. Thus, the air in the ATAL is a mixture of air masses coming from different atmospheric altitude layers. In addition, contributions from the model boundary layer originate in different geographic source regions. The location of the strongest updraft along the backward trajectories reveals a cluster of strong upward transport at the southern edge of the Himalayan foothills. From the top of the convective outflow level (about 13 km; 360 K) the air parcels ascend slowly to ATAL altitudes within a large-scale upward spiral driven by the diabatic heating in the anticyclonic flow of the South Asian summer monsoon at UTLS altitudes. Cases with a strong ATAL typically show boundary layer contributions from the Tibetan Plateau, the foothills of the Himalayas and other continental regions below the Asian monsoon. Weaker ATAL cases show higher contributions from the maritime boundary layer, often related to tropical cyclones, indicating a mixing of clean maritime and polluted continental air. On the one hand increasing anthropogenic emissions in the future are expected due to the strong growth of Asian economies; on the other hand the implementation of new emission control measures (in particular in China) has reduced the anthropogenic emissions of some pollutants contributing to the ATAL substantially. It needs to be monitored in the future whether the thickness and intensity of the ATAL will further increase, which will likely impact the surface climate.

Wildfire smoke in the lower stratosphere identified by in situ CO observations

Abstract. Wildfires emit large quantities of aerosols and trace gases, which occasionally reach the lower stratosphere. In August 2017, several pyro-cumulonimbus events injected a large amount of smoke into the stratosphere, observed by lidar and satellites. Satellite observations are in general the main method of detecting these events since in situ aircraft- or balloon-based measurements of atmospheric composition at higher altitudes are not made frequently enough. This work presents accidental balloon-borne trace gas observations of wildfire smoke in the lower stratosphere, identified by enhanced CO mole fractions at approximately 13.6 km. In addition to CO mole fractions, CO2 mole fractions and isotopic composition of CO (δ13C and δ18O) have been measured in air samples, from both the wildfire plume and background, collected using an AirCore and a lightweight stratospheric air sampler (LISA) flown on a weather balloon from Sodankylä (4–7 September 2017; 67.37∘ N, 26.63∘ E; 179 m a.m.s.l.), Finland. The greenhouse gas enhancement ratio (ΔCO:ΔCO2) and the isotopic signature based on δ13C(CO) and δ18O(CO) independently identify wildfire emissions as the source of the stratospheric CO enhancement. Back-trajectory analysis was performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS), tracing the smoke's origin to wildfires in British Columbia with an injection date of 12 August 2017. The trajectories are corrected for vertical displacement due to heating of the wildfire aerosols, by observations made by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument. Knowledge of the age of the smoke allowed for a correction of the enhancement ratio, ΔCO:ΔCO2, for the chemical removal of CO by OH. The stable isotope observations were used to estimate the amount of tropospheric air in the plume at the time of observation to be about 45±21 %. Finally, the plume extended over 1 km in altitude, as inferred from the observations.

Long-term variations in ozone levels in the troposphere and lower stratosphere over Beijing: observations and model simulations

Abstract. Tropospheric ozone is both a major pollutant and a short-lived greenhouse gas and has therefore caused much concern in recent years. The ozone profile in the troposphere and lower stratosphere over Beijing has been observed since 2002 by ozonesondes developed by the Institute of Atmospheric Physics. Increasing concentrations of tropospheric ozone from 2002 to 2010 measured by these balloon-based observations have been reported previously. As more observations are now available, we used these data to analyse the long-term variability of ozone over Beijing during the whole period from 2002 to 2018. The ozonesondes measured increasing concentrations of ozone from 2002 to 2012 in both the troposphere and lower stratosphere. There was a sudden decrease in observed ozone between 2011 and 2012. After this decrease, the increasing trend in ozone concentrations slowed down, especially in the mid-troposphere, where the positive trend became neutral. We used the Chemical Lagrangian Model of the Stratosphere (CLaMS) to determine the influence of the transport of ozone from the stratosphere to the troposphere on the observed ozone profiles. CLaMS showed a weak increase in the contribution of stratospheric ozone before the decrease in 2011–2012 and a much more pronounced decrease after this time. Because there is no tropospheric chemistry in CLaMS, the sudden decrease simulated by CLaMS indicates that a smaller downward transport of ozone from the stratosphere after 2012 may explain a significant part of the observed decrease in ozone in the mid-troposphere and lower stratosphere. However, the influence of stratospheric ozone in the lower troposphere is negligible in CLaMS, and the hiatus in the positive trend after 2012 can be attributed to a reduction in ozone precursors as a result of stronger pollution control measures in Beijing.

A convolution of observational and model data to estimate age of air spectra in the northern hemispheric lower stratosphere

Abstract. Derivation of mean age of air (AoA) and age spectra from atmospheric measurements remains a challenge and often requires output from atmospheric models. This study tries to minimize the direct influence of model output and presents an extension and application of a previously established inversion method to derive age spectra from mixing ratios of long- and short-lived trace gases. For a precise description of cross-tropopause transport processes, the inverse method is extended to incorporate air entrainment into the stratosphere across the tropical and extratropical tropopause. We first use simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS) to provide a general proof of concept of the extended principle in a controllable and consistent environment, where the method is applied to an idealized set of 10 trace gases with predefined constant lifetimes and compared to reference model age spectra. In the second part of the study we apply the extended inverse method to atmospheric measurements of multiple long- and short-lived trace gases measured aboard the High Altitude and Long Range (HALO) research aircraft during the two research campaigns POLSTRACC–GW-LCYCLE–SALSA (PGS) and Wave-driven Isentropic Exchange (WISE). As some of the observed species undergo significant loss processes in the stratosphere, a Monte Carlo simulation is introduced to retrieve age spectra and chemical lifetimes in stepwise fashion and to account for the large uncertainties. Results show that in the idealized model scenario the inverse method retrieves age spectra robustly on annual and seasonal scales. The extension to multiple entry regions proves reasonable as our CLaMS simulations reveal that in the model between 50 % and 70 % of air in the lowermost stratosphere has entered through the extratropical tropopause (30–90∘ N and S) on annual average. When applied to observational data of PGS and WISE, the method derives age spectra and mean AoA with meaningful spatial distributions and quantitative range, yet large uncertainties. Results indicate that entrainment of fresh tropospheric air across both the extratropical and tropical tropopause peaked prior to both campaigns, but with lower mean AoA for WISE than PGS data. The ratio of moments for all retrieved age spectra for PGS and WISE is found to range between 0.52 and 2.81 years. We conclude that the method derives reasonable and consistent age spectra using observations of chemically active trace gases. Our findings might contribute to an improved assessment of transport with age spectra in future studies.

Dehydration and low ozone in the tropopause layer over the Asian monsoon caused by tropical cyclones: Lagrangian transport calculations using ERA-Interim and ERA5 reanalysis data

Abstract. Low ozone and high water vapour mixing ratios are common features in the Asian summer monsoon (ASM) anticyclone; however, low ozone and low water vapour values were observed near the tropopause over Kunming, China, within the ASM using balloon-borne measurements performed during the SWOP (sounding water vapour, ozone, and particle) campaign in August 2009 and 2015. Here, we investigate low ozone and water vapour signatures in the upper troposphere and lower stratosphere (UTLS) using FengYun-2D, FengYun-2G, and Aura Microwave Limb Sounder (MLS) satellite measurements and backward trajectory calculations. Trajectories with kinematic and diabatic vertical velocities were calculated using the Chemical Lagrangian Model of the Stratosphere (CLaMS) trajectory module driven by both ERA-Interim and ERA5 reanalysis data. All trajectory calculations show that air parcels with low ozone and low water vapour values in the UTLS over Kunming measured by balloon-borne instruments originate from the western Pacific boundary layer. Deep convection associated with tropical cyclones over the western Pacific transports ozone-poor air from the marine boundary layer to the cold tropopause region. Subsequently, these air parcels are mixed into the strong easterlies on the southern side of the Asian summer monsoon anticyclone. Air parcels are dehydrated when passing the lowest temperature region (< 190 K) at the convective outflow of tropical cyclones. However, trajectory calculations show different vertical transport via deep convection depending on the employed reanalysis data (ERA-Interim, ERA5) and vertical velocities (diabatic, kinematic). Both the kinematic and the diabatic trajectory calculations using ERA5 data show much faster and stronger vertical transport than ERA-Interim primarily because of ERA5's better spatial and temporal resolution, which likely resolves convective events more accurately. Our findings show that the interplay between the ASM anticyclone and tropical cyclones has a significant impact on the chemical composition of the UTLS during summer.

Nitrification of the lowermost stratosphere during the exceptionally cold Arctic winter 2015–2016

Abstract. The Arctic winter 2015–2016 was characterized by exceptionally low stratospheric temperatures, favouring the formation of polar stratospheric clouds (PSCs) from mid-December until the end of February down to low stratospheric altitudes. Observations by GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) on HALO (High Altitude and LOng range research aircraft) during the PGS (POLSTRACC–GW-LCYCLE II–SALSA) campaign from December 2015 to March 2016 allow the investigation of the influence of denitrification on the lowermost stratosphere (LMS) with a high spatial resolution. Two-dimensional vertical cross sections of nitric acid (HNO3) along the flight track and tracer–tracer correlations derived from the GLORIA observations document detailed pictures of wide-spread nitrification of the Arctic LMS during the course of an entire winter. GLORIA observations show large-scale structures and local fine structures with enhanced absolute HNO3 volume mixing ratios reaching up to 11 ppbv at altitudes of 13 km in January and nitrified filaments persisting until the middle of March. Narrow coherent structures tilted with altitude of enhanced HNO3, observed in mid-January, are interpreted as regions recently nitrified by sublimating HNO3-containing particles. Overall, extensive nitrification of the LMS between 5.0 and 7.0 ppbv at potential temperature levels between 350 and 380 K is estimated. The GLORIA observations are compared with CLaMS (Chemical Lagrangian Model of the Stratosphere) simulations. The fundamental structures observed by GLORIA are well reproduced, but differences in the fine structures are diagnosed. Further, CLaMS predominantly underestimates the spatial extent of HNO3 maxima derived from the GLORIA observations as well as the overall nitrification of the LMS. Sensitivity simulations with CLaMS including (i) enhanced sedimentation rates in case of ice supersaturation (to resemble ice nucleation on nitric acid trihydrate (NAT)), (ii) a global temperature offset, (iii) modified growth rates (to resemble aspherical particles with larger surfaces) and (iv) temperature fluctuations (to resemble the impact of small-scale mountain waves) slightly improved the agreement with the GLORIA observations of individual flights. However, no parameter could be isolated which resulted in a general improvement for all flights. Still, the sensitivity simulations suggest that details of particle microphysics play a significant role for simulated LMS nitrification in January, while air subsidence, transport and mixing become increasingly important for the simulated HNO3 distributions towards the end of the winter.