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Every year during the Asian summer monsoon season from about mid-June to early September, a stable anticyclonic circulation system forms over the Himalayans. This Asian summer monsoon (ASM) anticyclone has been shown to promote transport of air into the stratosphere from the Asian troposphere, which contains large amounts of anthropogenic pollutants. Essential details of Asian monsoon transport, such as the exact time scales of vertical transport, the role of convection in cross-tropopause exchange, and the main location and level of export from the confined anticyclone to the strato sphere are still not fully resolved. Recent airborne observations from campaigns near the ASM anticyclone edge and centre in 2016 and 2017 respectively show a steady decrease in carbon monoxide (CO) and increase in ozone (O3) with height starting from tropospheric values of 80-100 ppb CO and 30-50 ppb O3 at about 365 K potential temperature. CO mixing ratios reach stratospheric background values of ~20 ppb at about 420 K and do not show a significant vertical gradient at higher levels, while ozone continues to increase throughout the altitude range of the aircraft measurements. Nitrous oxide (N2O) remains at or only marginally below its 2017 tropospheric mixing ratio of 326 ppb up to about 400 K, which is above the local tropopause. A decline in N2O mixing ratios that indicates a significant contribution of stratospheric air is only visible above this level. Based on our observations, we draw the following picture of vertical transport and confinement in the ASM anticyclone: rapid convective uplift transports air to near 16 km in altitude, corresponding to potential temperatures up to about 370 K. Although this main convective outflow layer extends above the level of zero radiative heating (LZRH), our observations of CO concentration show little to no evidence of convection actually penetrating the tropopause. Rather, further ascent occurs more slowly, consistent with isentropic vertical velocities of 0.3 - 0.8 K day-1. For gases not subject to microphysical processes, neither the lapse rate tropopause (LRT) around 380 K nor the cold point tropopause (CPT) around 390 K marks the strong discontinuity of the key tracers (CO, O3, and N2O). Up to about 10 to 20 K above the CPT, isolation of air inside the ASM anticyclone prevents significant in-mixing of stratospheric air. The observed changes in CO and O3 likely result from in-situ chemical processing. Above about 420 K, mixing processes become more significant and the air inside the anticyclone is exported vertically and horizontally into the surrounding stratosphere. [ABSTRACT FROM AUTHOR]

The Asian Summer Monsoon (ASM) traps convectively-lifted boundary layer pollutants inside its upper-tropospheric lower-stratospheric Asian monsoon anticyclone (AMA). It is associated with a seasonal and spatially-confined enhanced aerosol layer, called the Asian Tropopause Aerosol Layer (ATAL). The knowledge of the ATAL properties in terms of aerosol budget, chemical composition, as well as its variability and temporal trend is still largely uncertain, due to the dynamical variability of the AMA, the dearth of in situ observations in this region, the complex transport pathways of pollutants and its atmospheric chemical processes. In this work, we use the Community Earth System Model (CESM 1.2 version) based on the coupling of the Community Atmosphere Model (CAM5) and the MAM7 (Modal Aerosol Model) aerosol module to simulate the composition of the ATAL and its decadal trends. Our simulations cover a long-term period of 16 years from 2000 to 2015. We identify a double-peak aerosols vertical profile for the ATAL. We attribute the upper peak (around 100 hPa, predominant during early ATAL in June) to dry aerosols, possibly from nucleation processes and the lower peak (around 250 hPa, predominant for a well-developed and late ATAL, in July and August) to cloud-borne aerosols associated with convective clouds. We find that mineral dust is the dominant aerosol by mass in the ATAL showing a large interannual variability, but no long-term trend, due to its natural variation. The results between 120-80 hPa (dry aerosol peak) suggest that for aerosols other than dust the ATAL is composed of around 40 % of sulfate, 30% of secondary and 15 % of primary organic aerosols, 14 % of ammonium aerosols and less than 3 % of black carbon. The analysis of the anthropogenic and biomass burning aerosols shows a positive trend for all aerosols simulated by CESM-MAM7. [ABSTRACT FROM AUTHOR]

In June 2019 a stratospheric moderate eruption occurred at Raikoke (48° N, 153° E). Satellite observations show the injection of ash and SO2 into the lower stratosphere and an early entrainment of the plume into a cyclone. Following the Raikoke eruption stratospheric Aerosol Optical Depth (sAOD) values increased in the whole northern hemisphere and tropics and remained enhanced for more than one year, with peak values at 0.040 (shorter-wavelength visible, higher northern latitudes) to 0.025 (shorter-wavelength visible, average northern hemisphere). Discrepancies between observations and models indicate that ash has played a role on evolution and sAOD values. Top of the atmosphere radiative forcings are estimated at values between -0.3 and -0.4 W/m² (clear-sky), and of -0.1 to -0.2 W/m² (all-sky), comparable to what was estimated for the Sarychev eruption in 2009. Almost simultaneously two significantly smaller stratospheric eruptions occurred at Ulawun (5° S, 151° E) in June and August. Aerosol enhancements from the Ulawun eruptions had mainly an impact on the tropics and southern hemisphere. The Ulawun plume circled the Earth within one month in the tropics. Peak shorter- wavelength sAOD values at 0.01 are found in the tropics following the Ulawun eruptions, and a radiative forcing not exceeding -0.15 (clear-sky) and -0.05 (all-sky). Compared to the Canadian Fires (2017), Ambae eruption (2018), Ulawun (2019) and the Australian fires (2019/2020) highest sAOD values and RF are found for the Raikoke eruption. [ABSTRACT FROM AUTHOR]

The StratoClim airborne campaign took place in Nepal from 27 July to 10 August 2017 to document the physical and chemical properties of the South Asian Upper Troposphere Lower Stratosphere (UTLS) during the Asian Summer Monsoon (ASM). In the present paper, simulations with the Meso-NH cloud-chemistry model at a horizontal resolution of 15 km are performed over the Asian region to characterize the impact of monsoon deep convection on the composition of Asian Monsoon Anticyclone (AMA) and on the formation of the Asian Tropopause Aerosol Layer (ATAL) during the StratoClim campaign. StratoClim took place during a break phase of the monsoon with an intense convective activity over south China and Sichuan. Comparisons between Brightness Temperature (BT) at 10.8 microns observed by satellite sensors and simulated by Meso-NH highlight the ability of the model to correctly reproduce the life cycle of deep convective clouds. Comparison between CO and O3 concentrations from Meso-NH and airborne observations (StratoClim and IAGOS) demonstrates that the model captures most of the observed variabilities. Nevertheless, for both gases, the model tends to overestimate the concentrations and misses some thin CO plumes related to local convective events probably because of a too coarse resolution, but the convective uplift of pollution is very well captured by the model. We have therefore focused on the impact of Sichuan convection on the AMA composition. A dedicated sensitivity simulation showed that the 7 August convective event brought large amounts of CO deep into the AMA and even across the 380 K isentropic level located at 17.8 km. This Sichuan contribution enhanced the CO concentration by ~15 % to reach more than 180 ppbv over a large area around 15 km height. Noteworthy, Meso-NH captures the impact of the diluted Sichuan plume on the CO concentration during a StratoClim flight south of Kathmandu highlighting its ability to reproduce the transport pathway of Sichuan pollution. According to the model, primary organic aerosol and black carbon particles originating from Sichuan are transported following the same pathway as CO. The large particles are heavily scavenged within the precipitating part of the convective clouds but remain the most important contributor to the particle mass in the AMA. Over the whole AMA region, the 7 August convective event resulted in a 0.5% increase of CO over the 10-20 km range that lasted about 2 days. The impact of pollution uplift from three regions (India, China and Sichuan) averaged over the first 10 days of August has also been evaluated with sensitivity simulations. Even during this monsoon break phase, the results confirm the predominant role of India relative to China with respective contributions of 11 and 7 % to CO in the 10[sup -1]5 km layer. Moreover, during this period a large part (35 %) of the Chinese contribution comes from the Sichuan basin alone. [ABSTRACT FROM AUTHOR]

We show that a fire plume originating at high northern latitudes during the Canadian wildfire event in July/August 2017 reached the tropics, and subsequently the tropical stratosphere via the ascending branch of the Brewer-Dobson Circulation (BDC). The transport from high to low latitudes in the upper troposphere and lowermost stratosphere was mediated by the anticyclonic flow of the Asian monsoon circulation. The fire plume reached the Asian monsoon area in late August/early September, when the Asian Monsoon Anticyclone (AMA) was still in place. While there is no evidence of mixing into the center of the AMA, we show that a substantial part of the fire plume is entrained into the anticyclonic flow at the AMA edge, and is transported into the tropical Upper-Troposphere–Lower-Stratosphere (UTLS), and possibly the Southern Hemisphere particularly following the north-south flow on the eastern side. In the tropics the fire plume is lifted by ~1.5 km per month. Inside the AMA we find evidence of the Asian Tropopause Aerosol Layer (ATAL) in August, doubling background aerosol conditions with a calculated top of the atmosphere shortwave radiative forcing (RF) of −0.05 W/m2. The regional climate impact of the fire signal in the wider Asian monsoon area in September exceeds the impact of the ATAL by a factor of 2–4 and compares to that of a plume coming from an advected moderate volcanic eruption. The stratospheric, trans-continental transport of this plume to the tropics and the related regional climate impact point at the importance of long-range dynamical interconnections of pollution sources. [ABSTRACT FROM AUTHOR]

When computing climatological averages of atmospheric trace gas mixing ratios obtained from satellite-based measurements, sampling biases arise if data coverage is not uniform in space and time. Complete homogeneous spatio-temporal coverage is essentially impossible to achieve. Solar occultation measurements, by virtue of satellite orbits and the requirement of direct observation of the sun through the atmosphere, result in particularly sparse spatial coverage. In this study, a method is presented to adjust for such sampling biases when calculating climatological means. The method is demonstrated using carbonyl sulfide (OCS) measurements at 16km altitude from the ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform 15 Spectrometer). At this altitude, OCS mixing ratios show a steep gradient between the poles and equator. ACE-FTS measurements, which are provided as vertically resolved profiles, and integrated stratospheric OCS columns are used in this study. The bias adjustment procedure requires no additional observations other than the satellite data product itself and is expected to be generally applicable when constructing climatologies of long-lived tracers from sparsely and heterogeneously sampled satellite data. In a first step of the adjustment procedure, a regression model is used to fit a 2-D surface to all available ACE-FTS OCS measurements as a function of day-of-year and latitude. The regression model fit is used to calculate an adjustment factor, 20 which is then used to adjust each measurement individually. The mean of the adjusted measurement points of a chosen spatio-temporal frame is then used as the bias-free climatological value. When applying the adjustment factor to seasonal averages in 30° zones, the maximum spatio-temporal sampling bias adjustment was 11% for OCS mixing ratios at 16km and 5% for the stratospheric OCS column. The adjustments were validated against the much denser and more homogeneous OCS data product from the limb-sounding MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) instrument, and both the direction and sign of the adjustments were in agreement with the adjustment of the ACE-FTS data. [ABSTRACT FROM AUTHOR]

The climate active trace-gas carbonyl sulfide (OCS) is the most abundant sulfur gas in the atmosphere. A missing source in its atmospheric budget is currently suggested, resulting from an upward revision of the vegetation sink in top-down approaches. Oceanic emissions have been proposed to close the resulting gap in the atmospheric budget. We present a bottom-up approach including new observations of OCS in surface waters of the tropical Atlantic, Pacific and Indian oceans to show that direct OCS emissions are insufficient to account for the missing source. Extrapolation of our observations using a biogeochemical box model suggests oceanic net uptake instead of emission for the entire tropical ocean area and, further, a global ocean source strength well below that suggested by top-down estimates. This bottom-up estimate of oceanic emissions has implications for using OCS as a proxy for terrestrial CO2 uptake, which is currently hampered by the inadequate quantification of atmospheric OCS sources and sinks. [ABSTRACT FROM AUTHOR]

The UTLS is characterized by significant gradients in trace gas mixing ratios that arise fromi) mixing of different fractions of tropospheric and stratospheric air and ii) photochemicalprocessing as air rises from the troposphere to the stratosphere (particularly in the tropics).We use satellite and in-situ measurements of two different tracers to investigate theseprocesses in the region of the Asian Monsoon Anticyclone (AMA): carbon monoxide (CO)and carbonyl sulfide (OCS). CO is a short-lived tracer with a photochemical lifetime of ∼1 – 4 months. CO mixingratios are sensitive to both photochemical depletion and inmixing of stratospheric air masses.OCS, on the other hand, can be regarded as photochemically inert in the UTLS (significantphotochemical destruction of OCS takes place only in the tropical pipe above ∼ 22 kmaltitude). Therefore, OCS is sensitive only to stratospheric inmixing. Based on observedvertical profiles of the two gases in different positions relative to the core of the AMA, we settwo hypotheses: In and directly above the AMA core, the composition is dominated by photochemical processing Further away from the AMA core, mixing processes become more important.This implies significant active net transport/ascend of upper tropospheric air into thestratosphere close to the AMA core and a more bi-directional transport regime elsewhere. [ABSTRACT FROM AUTHOR]

We show that a fire plume originating at high northern latitudes during the Canadian wild fireevent in July/August 2017 reached the tropics, and subsequently the stratosphere via theascending branch of the Brewer-Dobson-Circulation (BDC). For this, we use a combinationof aerosol extinction data from the Stratospheric Aerosol and Gas Experiment III (SAGEIII)and the Ozone Mapping Profiler Suite (OMPS), carbon dioxide measurements from theInfrared Atmospheric Sounding Interferometer (IASI), FLEXPART-TRACZILLAback-trajectories and information for the position and strength of the Asian MonsoonAnticyclone (AMA) transport barrier from the Chemical Lagrangian Model of theStratosphere (CLaMS). The transport from high to low latitudes in the upper troposphere andlowermost stratosphere was mediated by the anticyclonic flow of the Asian monsooncirculation. The Canadian fire plume reached the Asian monsoon area in late August/earlySeptember, when the AMA was still in place. While there is no evidence of systematicmixing into the center of the AMA, we show that a substantial part of the Canadian fire plumeis entrained into the circulation at the AMA edge, and is transported into the tropicalUTLS, and possibly the Southern Hemisphere particularly following the North-Southflow on the eastern side. In the tropics the fire plume is lifted by about 1.5 km permonth. Inside the AMA we find evidence of the Asian Tropopause Aerosol Layer (ATAL) inAugust, doubling background aerosol conditions with a top of the atmosphere shortwaveradiative forcing of -0.05 W/m2. This is estimated using the UVSPEC radiative transfermodel and the LibRadtran package. The regional climate impact of the fire signal in the widerAsian monsoon area in September exceeds the impact of the ATAL by a factorof ∼3 (-0.13W/m2). Once in the stratosphere, the climate impact of such kind oftrans-continental transported plumes can be hemispheric and long-lasting, pointing atthe importance of this long-range dynamical interconnection of pollution sources. [ABSTRACT FROM AUTHOR]