Comment on acp-2021-905

<p>Air mass transport within the summertime Asian monsoon circulation provides a major source of anthropogenic pollution for the upper troposphere and lower stratosphere (UTLS). In our study, we investigate the quasi-horizontal transport of airmasses 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 for frequent summertime transport from the monsoon anticyclone to mid-latitudes over the North Pacific, even reaching high latitude regions of Siberia and Alaska. Particularly, the most promising region and time for measurements of transported anticyclonic air masses that cross the tropopause, is the North Pacific from July to August. Most of the low–PV cutoffs related to air masses exported from the ASMA have lifetimes shorter than one week (about 90%) and sizes smaller than 1 percent of the northern hemisphere (NH) area. The chemical composition of these air masses is characterised 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 characteristics of the monsoon anticyclone to characteristics of the lower stratospheric background during about one week, indicating continuous mixing with the background atmosphere.</p>

Airborne in situ measurements of short-lived chlorocarbons and investigation of their pathways from northern hemispheric source regions into the lowermost stratosphere

Abstract. Eastward air-mass transport from the Asian summer monsoon (ASM) anticyclone in the upper troposphere and lower stratosphere (UTLS) often involves eastward-shedding vortices, which can cover most of the Japanese archipelago. We investigated the aerosol characteristics of these vortices by analysing data from two lidar systems in Japan, at Tsukuba (36.1∘ N, 140.1∘ E) and Fukuoka (33.55∘ N, 130.36∘ E), during the summer of 2018. We observed several events with enhanced particle signals at Tsukuba at 15.5–18 km of altitude (at or above the local tropopause) during August–September 2018, with a backscattering ratio of ∼ 1.10 and particle depolarization of ∼ 5 % (i.e. not spherical, but more spherical than ice crystals). These particle characteristics may be consistent with those of solid aerosol particles, such as ammonium nitrate. Each event had a timescale of a few days. During the same study period, we also observed similar enhanced particle signals in the lower stratosphere at Fukuoka. The upper troposphere is often covered by cirrus clouds at both lidar sites. Backward trajectory calculations for these sites for days with enhanced particle signals in the lower stratosphere and days without indicate that the former air masses originated within the ASM anticyclone and the latter more from edge regions. Reanalysis carbon monoxide and satellite water vapour data indicate that eastward-shedding vortices were involved in the observed aerosol enhancements. Satellite aerosol data confirm that the period and latitudinal region were free from the direct influence of documented volcanic eruptions and high-latitude forest fires. Our results indicate that the Asian tropopause aerosol layer (ATAL) over the ASM region extends east towards Japan in association with the eastward-shedding vortices and that lidar systems in Japan can detect at least the lower-stratospheric portion of the ATAL during periods when the lower stratosphere is undisturbed by volcanic eruptions and forest fires. The upper-tropospheric portion of the ATAL is either depleted by tropospheric processes (convection and wet scavenging) during eastward transport or is obscured by much stronger cirrus cloud signals.

<strong class="journal-contentHeaderColor">Abstract.</strong> <span id="page2050"/>Efficient transport pathways for ozone-depleting very short-lived substances (VSLSs) from their source regions into the stratosphere are a matter of current scientific debate; however they have yet to be fully identified on an observational basis. Understanding the increasing impact of chlorine-containing VSLSs (Cl-VSLSs) on stratospheric ozone depletion is important in order to validate and improve model simulations and future predictions. We report on a transport study using airborne in situ measurements of the Cl-VSLSs dichloromethane (CH<span class="inline-formula">₂</span>Cl<span class="inline-formula">₂</span>) and trichloromethane (chloroform, CHCl<span class="inline-formula">₃</span>) to derive a detailed description of two transport pathways from (sub)tropical source regions into the extratropical upper troposphere and lower stratosphere (Ex-UTLS) in the Northern Hemisphere (NH) late summer. The Cl-VSLS measurements were obtained in the upper troposphere and lower stratosphere (UTLS) above western Europe and the midlatitude Atlantic Ocean in the frame of the WISE (Wave-driven ISentropic Exchange) aircraft campaign in autumn 2017 and are combined with the results from a three-dimensional simulation of a Lagrangian transport model as well as back-trajectory calculations. Compared to background measurements of similar age we find up to <span class="inline-formula">150</span> % enhanced CH<span class="inline-formula">₂</span>Cl<span class="inline-formula">₂</span> and up to <span class="inline-formula">100</span> % enhanced CHCl<span class="inline-formula">₃</span> mixing ratios in the extratropical lower stratosphere (Ex-LS). We link the measurements of enhanced CH<span class="inline-formula">₂</span>Cl<span class="inline-formula">₂</span> and CHCl<span class="inline-formula">₃</span> mixing ratios to emissions in the region of southern and eastern Asia. Transport from this area to the Ex-LS at potential temperatures in the range of 370–400 K takes about 6–11 weeks via the Asian summer monsoon anticyclone (ASMA). Our measurements suggest anthropogenic sources to be the cause of these strongly elevated Cl-VSLS concentrations observed at the top of the lowermost stratosphere (LMS). A faster transport pathway into the Ex-LS is derived from particularly low CH<span class="inline-formula">₂</span>Cl<span class="inline-formula">₂</span> and CHCl<span class="inline-formula">₃</span> mixing ratios in the UTLS. These low mixing ratios reflect weak emissions and a local seasonal minimum of both species in the boundary layer of Central America and the tropical Atlantic. We show that air masses uplifted by hurricanes, the North American monsoon, and general convection above Central America into the tropical tropopause layer to potential temperatures of about 360–370 K are transported isentropically within 5–9 weeks from the boundary layer into the Ex-LS. This transport pathway linked to the North American monsoon mainly impacts the middle and lower part of the LMS with particularly low CH<span class="inline-formula">₂</span>Cl<span class="inline-formula">₂</span> and CHCl<span class="inline-formula">₃</span> mixing ratios. In a case study, we specifically analyze air samples directly linked to the uplift by the Category 5 Hurricane Maria that occurred during October 2017 above the Atlantic Ocean. CH<span class="inline-formula">₂</span>Cl<span class="inline-formula">₂</span> and CHCl<span class="inline-formula">₃</span> have similar atmospheric sinks and lifetimes, but the fraction of biogenic emissions is clearly higher for CHCl<span class="inline-formula">₃</span> than for the mainly anthropogenically emitted CH<span class="inline-formula">₂</span>Cl<span class="inline-formula">₂</span>; consequently lower CHCl<span class="inline-formula">₃</span> : CH<span class="inline-formula">₂</span>Cl<span class="inline-formula">₂</span> ratios are expected in air parcels showing a higher impact of anthropogenic emissions. The observed CHCl<span class="inline-formula">₃</span> : CH<span class="inline-formula">₂</span>Cl<span class="inline-formula">₂</span> ratio suggests clearly stronger anthropogenic emissions in the region of southern and eastern Asia compared to those in the region of Central America and the tropical Atlantic. Overall, the transport of strongly enhanced CH<span class="inline-formula">₂</span>Cl<span class="inline-formula">₂</span> and CHCl<span class="inline-formula">₃</span> mixing ratios from southern and eastern Asia via the ASMA is the main factor in increasing the chlorine loading from the analyzed VSLSs in the Ex-LS during the NH late summer. Thus, further increases in Asian CH<span class="inline-formula">₂</span>Cl<span class="inline-formula">₂</span> and CHCl<span class="inline-formula">₃</span> emissions, as frequently reported in recent years, will further increase the impact of Cl-VSLSs on stratospheric ozone depletion.

Abstract. In the frame of the SWOP (sounding water vapour, ozone, and particle) campaign during the Asian summer monsoon (ASM), ozone and water vapour profiles were measured by balloon-borne sensors launched from Lhasa (29.66° N, 91.14° E, elevation 3650 m), China, in August 2013. In total, 24 soundings were launched, nearly half of which show strong variations in the relationship between ozone and water vapour in the tracer–tracer correlation in the upper troposphere and lower stratosphere (UTLS). For each sounding, 20-day backward trajectories were calculated using the trajectory module of the Chemical Lagrangian Model of the Stratosphere (CLaMS) to analyse these variations. The trajectory calculations demonstrate that three tropical cyclones (tropical storm Jebi, typhoons Utor and Trami), which occurred over the western Pacific Ocean during August 2013, had a considerable impact on the vertical distribution of ozone and water vapour by uplifting marine air masses to altitudes of the ASM anticyclone. Air parcels subsequently arrived at the observation site via two primary pathways: firstly via direct horizontal transport from the location of the typhoon to the station within approximately 3 days, and secondly via transport following the clockwise wind flow of the ASM within a timescale of 1 week. Furthermore, the interplay between the spatial position of the ASM anticyclone and tropical cyclones plays a key role in controlling the transport pathways of air parcels from the boundary layer of the western Pacific to Lhasa in horizontal and vertical transport. Moreover, the statistical analysis shows that the strongest impact by typhoons is found at altitudes between 14.5 and 17 km (365–375 K). Low ozone values (50–80 ppbv) were observed between 370 and 380 K due to the strong vertical transport within tropical cyclones.

Abstract. We have performed backward trajectory calculations and simulations with the three-dimensional Chemical Lagrangian Model of the Stratosphere (CLaMS) for two succeeding monsoon seasons using artificial tracers of air mass origin. With these tracers we trace back the origin of young air masses (age &lt;6 months) at the top of the Asian monsoon anticyclone and of air masses within the tropical pipe (6 months &lt; age &lt;18 months) during summer 2008. The occurrence of young air masses (&lt;6 months) at the top of the Asian monsoon anticyclone up to ∼460 K is in agreement with satellite measurements of chlorodifluoromethane (HCFC-22) by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument. HCFC-22 can be considered as a regional tracer for continental eastern Asia and the Middle East as it is mainly emitted in this region. Our findings show that the transport of air masses from boundary layer sources in the region of the Asian monsoon into the tropical pipe occurs in three distinct steps. First, very fast uplift in “a convective range” transports air masses up to 360 K potential temperature within a few days. Second, air masses are uplifted from about 360 K up to 460 K within “an upward spiralling range” within a few months. The large-scale upward spiral extends from northern Africa to the western Pacific. The air masses are transported upwards by diabatic heating with a rate of up to 1–1.5 K per day, implying strong vertical transport above the Asian monsoon anticyclone. Third, transport of air masses occurs within the tropical pipe up to 550 K associated with the large-scale Brewer–Dobson circulation within ∼1 year. In the upward spiralling range, air masses are uplifted by diabatic heating across the (lapse rate) tropopause, which does not act as a transport barrier, in contrast to the extratropical tropopause. Further, in the upward spiralling range air masses from inside the Asian monsoon anticyclone are mixed with air masses convectively uplifted outside the core of the Asian monsoon anticyclone in the tropical adjacent regions. Moreover, the vertical transport of air masses from the Asian monsoon anticyclone into the tropical pipe is weak in terms of transported air masses compared to the transport from the monsoon anticyclone into the northern extratropical lower stratosphere. Air masses from the Asian monsoon anticyclone (India/China) contribute a minor fraction to the composition of air within the tropical pipe at 550 K (6 %), and the major fractions are from Southeast Asia (16 %) and the tropical Pacific (15 %).

&amp;lt;p&amp;gt;A robust but thin aerosol layer in summer extending geographically from Eastern Mediterranean to Western China, the Asian Tropopause Aerosol Layer (ATAL) was observed and verified by the CALIPSO lidar measurements. However, its source and forming mechanism is still under debate. In August 2018 and 2019, two experimental campaigns over the Tibetan Plateau were carried out at Golmud (GLM, 36.48&amp;amp;#176;N, 94.93&amp;amp;#176;E) and Qaidam (QDM, 37.74&amp;amp;#176;N, 95.34&amp;amp;#176;E), during which a balloon-borne Portable Optical Particle Counter (POPS) was used to measure the features of aerosol particulates. The in-situ measurements show a robust ATAL around the tropopause, ranging from 14 to 18 km a.s.l., with a maximum aerosol number density of 35&amp;amp;#8211;40 cm&amp;lt;sup&amp;gt;-3&amp;lt;/sup&amp;gt; and a maximum aerosol mass concentration of 0.13 &amp;amp;#956;g m&amp;lt;sup&amp;gt;-3&amp;lt;/sup&amp;gt; for particles with diameters between 0.12 and 3 &amp;amp;#956;m, and majority of the particulates (98%) are smaller than 0.4 &amp;amp;#956;m in diameter.&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;Backward-trajectory simulations are conducted with the Massive-Parallel Trajectory Calculations (MPTRAC) model to investigate the possible sources and transport pathways of the observed particulates. The backward-trajectory analysis revealed that the air parcels arrived at the altitude of the ATAL through two separate pathways: 1) the uplift below the 360 K isentropic surface, where air parcels were first elevated to the upper troposphere and then joined the ASM anticyclonic circulation, which will take about 5&amp;amp;#8211;10 days; and 2) the quasi-horizontal transport along the anticyclonic circulation, located approximately between the 360 and 440 K isentropic surfaces. The dispersion of the volcanic aerosol from the volcanic eruption of Raikoke in June 2019 has enhanced the aerosol layer in the Tibetan Plateau upper troposphere and lower stratosphere (UTLS), but the ATAL was not concealed by the volcanic plume because the boundary of the Asian summer monsoon (ASM) anticyclone acted as a transport barrier which stopped most of the volcanic aerosol entering the ASM region. Only at most 20% of the aerosol particulates observed in the Tibetan Plateau UTLS was contributed by the Raikoke volcanic eruption. Comparing with the Nabro eruption in 2011, the influence of volcanic eruption on the ATAL significantly depends on the relative geographical location of the volcanic eruption and the ASM anticyclone, as well as the volcanic plume height.&amp;lt;/p&amp;gt;

The summer monsoon anticyclones are the dominant climatological features of the Northern Hemispheric (NH) summertime circulation in the upper troposphere and lower stratosphere (UTLS). However, the response of these anticyclones to the increased levels of remains highly uncertain, as does the impact on the distribution of UTLS ozone and other tracers. This study examines the response of the NH summertime monsoon anticyclones and UTLS ozone to the abrupt increase in forcing using output from a suite of coupled ocean–atmosphere general circulation model simulations. These models show an equatorward shift of the Asian summer monsoon anticyclone, a weakening of the North American summer monsoon anticyclone, and a stronger westerly flow penetrating deep into the tropics above the Pacific Ocean and North America. We use additional idealized experiments from atmosphere‐only general circulation models with prescribed SSTs and sea ice concentration to isolate the direct atmospheric radiative effects from the indirect effect of SST warming on the UTLS monsoon anticyclones. Comparison between atmosphere‐only and coupled ocean–atmosphere experiments shows that SST warming is the principal mechanism producing UTLS monsoonal circulation changes. The experiments result in a significant reduction up to 40%–50% of the UTLS ozone in the northern tropics, which could have an impact on radiative balance near the surface.

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.

Abstract. Every year during the Asian summer monsoon season from about mid-June to early September, a stable anticyclonic circulation system forms over the Himalayas. 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 timescales 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 stratosphere 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 around 100 ppb CO and 30–50 ppb O3 at about 365 K potential temperature. CO mixing ratios reach stratospheric background values below ∼25 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 333 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 0.7–1.5 K d−1. For the key tracers (CO, O3, and N2O) in our study, none of which are subject to microphysical processes, neither the lapse rate tropopause (LRT) around 380 K nor the cold point tropopause (CPT) around 390 K marks a strong discontinuity in their profiles. Up to about 20 to 35 K above the LRT, isolation of air inside the ASM anticyclone prevents significant in-mixing of stratospheric air (throughout this text, the term in-mixing refers specifically to mixing processes that introduce stratospheric air into the predominantly tropospheric inner anticyclone). 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.

Defining the upper boundary of the Asian Tropopause Aerosol Layer (ATAL) using the static stability

There are two key modes of the South Asia high (SAH) during the boreal summer: the Iranian Plateau (IP) and Tibetan Plateau (TP) modes. The anomalies of chemical constituents in the upper troposphere and lower stratosphere (UTLS) region within the SAH area largely depend on this bimodality. To better understand the underlying mechanisms of this dependence, the ensemble of 30-day backward trajectories, initialized in the UTLS region within the SAH, was simulated by a Lagrangian model FLEXPART. The comparative diagnostic was performed from the perspective of atmospheric ventilation. The results show that vertical transport from the lower troposphere to the UTLS during the TP mode was very efficient, resulting in tropospheric air mass transported into the UTLS within a shorter timescale than during the IP mode. Furthermore, the effect of SAH isolation during the TP mode was stronger than during the IP mode. This stronger trapping is likely to force the tropospheric air mass to reside in the SAH area for a longer period of time. In addition, compared to the IP mode, near-surface air mass sources during the TP mode overlapped more with areas of severe air pollution (CO emissions). The above three factors associated with the processes of atmospheric ventilation, i.e., the efficiency of vertical transport, the strength of the SAH isolation, and the boundary layer sources, provide potential explanations as to why the anomalies of atmospheric constituents in the UTLS are different between the TP and the IP mode.

Simulations of the effects of deep convection on the structure of potential vorticity (PV) in the upper troposphere and lower stratosphere (UTLS) have shown that a common signature in the presence of ambient horizontal vorticity is a horizontal PV dipole. Here, the relationship between convection and PV structures in the UTLS in Tropical Cyclone Talas and the extratropical “Super Tuesday” cyclone is investigated with the University of Wisconsin Nonhydrostatic Modeling System (UWNMS). Dipoles of potential temperature in the UTLS are interpreted as an upward deflection of the ambient flow over the updraft (cold), followed by subsidence in its lee (warm), aligned with the wind direction. PV dipoles larger than ±20 PV units (1 PVU = 10−6 K kg−1 m2 s−1) are identified, with typical vertical and horizontal extents of ~3 and ~200 km, respectively, and lifetimes up to 12 h. Confirming the findings of Chagnon and Gray, it is found that horizontal PV dipoles are related to vortex tilting, where horizontally oriented vorticity associated with vertical shear of the ambient wind is bent into a horseshoe shape by the updraft, yielding a PV dipole. This suggests that theta dipoles are perpendicular to PV dipoles and that “low PV lies to the left of the wind shear,” or, in the case of tropical cyclones, “low PV lies radially outward.” Mesoscale jets occur between the dipoles, which oppose the ambient anticyclonic flow. During the extratropical transition of Talas, convective PV anomalies evolved under synoptic-scale deformation into a pair of PV streamers, which modified the midlatitude westerly jet.

Abstract. Numerous studies have presented evidence that the Asian summer monsoon anticyclone substantially influences the distribution of trace gases – including water vapour – in the upper troposphere and lower stratosphere (e.g. Santee et al., 2017). Stratospheric water vapour in turn strongly affects surface climate (see e.g. Solomon et al., 2010). Here, we analyse the characteristics of water vapour transport from the upper troposphere in the Asian monsoon region to the stratosphere employing a multiannual simulation with the chemistry-transport model CLaMS (Chemical Lagrangian Model of the Stratosphere). This simulation is driven by meteorological data from ERA-Interim and features a water vapour tagging that allows us to assess the contributions of different upper tropospheric source regions to the stratospheric water vapour budget. Our results complement the analysis of air mass transport through the Asian monsoon anticyclone by Ploeger et al. (2017). The results show that the transport characteristics for water vapour are mainly determined by the bulk mass transport from the Asian monsoon region. Further, we find that, although the relative contribution from the Asian monsoon region to water vapour in the deep tropics is rather small (average peak contribution of 14 % at 450 K), the Asian monsoon region is very efficient in transporting water vapour to this region (when judged according to its comparatively small spatial extent). With respect to the Northern Hemisphere extratropics, the Asian monsoon region is much more impactful and efficient regarding water vapour transport than e.g. the North American monsoon region (averaged maximum contributions at 400 K of 29 % versus 6.4 %).

The high elevation, complex topography, and unique atmospheric circulations of the Tibetan Plateau (TP) make its optical turbulence characteristics different from those in low-elevation regions. In this study, the characteristics of the atmospheric refractive index structure constant (Cn2) profiles in the Lhasa area at different strength states of the Asian summer monsoon anticyclone (ASMA) are analyzed based on precious in situ sounding data measured over the Lhasa in August 2018. Cn2 in the upper troposphere–lower stratosphere fluctuates significantly within a few days during the ASMA, particularly in the upper troposphere. The effect of the ASMA on Cn2 varies among the upper troposphere, tropopause, and lower stratosphere. The stronger and closer the ASMA is to Lhasa, the more pronounced is the “upper highs and lower lows” pressure field structure, which is beneficial for decreasing the potential temperature lapse rate. The decrease in static stability is an important condition for developing optical turbulence, elevating the tropopause height, and reducing the tropopause temperature. However, if strong high-pressure activity occurs at the lower pressure layer, such as at 500 hPa, an “upper highs and lower highs” pressure field structure forms over the Lhasa, increasing the potential temperature lapse rate and suppressing the convective intensity. Being almost unaffected by low-level atmospheric high-pressure activities, the ASMA, as the main influencing factor, mainly inhibits Cn2 in the tropopause and lower stratosphere. The variations of turbulence intensity in UTLS caused by ASMA activities also have a great influence on astronomical parameters, which will have certain guiding significance for astronomical site testing and observations.