Asian Tropopause Aerosol Layer Research Articles

Characterization of refractory aerosol particles collected in the tropical upper troposphere–lower stratosphere (UTLS) within the Asian tropopause aerosol layer (ATAL)

Abstract. Aerosol particles with diameters larger than 40 nm were collected during the flight campaign StratoClim 2017 within the Asian tropopause aerosol layer (ATAL) of the 2017 monsoon anticyclone above the Indian subcontinent. A multi-impactor system was installed on board the aircraft M-55 Geophysica, which was operated from Kathmandu, Nepal. The size and chemical composition of more than 5000 refractory particles/inclusions of 17 selected particle samples from seven different flights were analyzed by use of scanning electron microscopy (SEM) and transmission electron microscopy (TEM) combined with energy dispersive X-ray (EDX) microanalysis. Based on chemical composition and morphology, the refractory particles were assigned to the following particle groups: extraterrestrial, silicates, Fe-rich, Al-rich, Hg-rich, other metals, C-rich, soot, Cl-rich, and Ca-rich. Most abundant particle groups within the refractory particles are silicates and C-rich (non-volatile organics). In samples taken above the tropopause, extraterrestrial particles are becoming increasingly important with rising altitude. The most frequent particle sources for the small (maximum in size distribution DP-max=120 nm) refractory particles carried into the ATAL are combustion processes at the ground (burning of fossil fuels/biomass burning) and the agitation of soil material. The refractory particles in the ATAL represent only a very small fraction (< 2 % by number for particles > 40 nm) of the total aerosol particles, which are dominated by species like ammonium, sulfate, nitrate, and volatile organics. During one flight, a large number of very small (DP-max=25 nm) cinnabar particles (HgS) were detected, which are supposed to originate from a ground source such as coal combustion or underground coal fires.

Reconsidering the Existence of a Trend in the Asian Tropopause Aerosol Layer (ATAL) From 1979 to 2017

AbstractAn enhanced aerosol layer, known as the Asian Tropopause Aerosol Layer (ATAL), has been observed within the seasonal Asian monsoon anticyclone (AMA) since the late 1990s. Given the apparently abrupt appearance of this layer based on observations, it has been speculated that it originates from increasing human made emissions in Asia. However, the ATAL confinement is a result of a dynamical feature and does not purely consist of human made components. We herein investigate the possible existence of an ATAL earlier than the late 1990s. We exploit earliest possible, high quality space‐based aerosol observations from Stratospheric Aerosol and Gas Experiment, or SAGE (1979–1981), SAGE III/ISS (2017, ongoing) and revisit SAGE II (1984–2005) data analysis. We find that seasonal averaged solar occultation aerosol measurements (past and present) can neither be used to exclude the existence of the ATAL, nor to infer a significant trend. However, first CAM5‐MAM7 simulations indicate the presence of an ATAL signal for the tested years 1979 and 1980, with a human made component. We hypothesize that the human made component of the ATAL likely occurred since at least the 1970s, while the natural ATAL component (e.g., from dust) has always existed. Extended simulation based ATAL evolution studies are therefore the most reliable source for early ATAL investigations.

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.

The South American Tropopause Aerosol Layer (SATAL)

Abstract The presence of an aerosol layer in the upper troposphere/lower stratosphere (UT/LS) in South America was identified with the Modern-Era Retrospective Analysis for Research and Applications version 2 (MERRA-2). This layer, which we shall refer to as the South American tropopause aerosol layer (SATAL), was identified over the Amazon basin at altitudes between 11 and 14 km. It exhibits a seasonal behavior similar to the Asian tropopause aerosol layer (ATAL) and the North American tropopause aerosol layer (NATAL). The SATAL is observed from October to March, coinciding with the presence of the South American monsoon. It forms first in the eastern Amazon basin in October, then moves to the southern Amazon, where it weakens in December–January and finally dissipates in February–March. We hypothesize that two main factors influence the SATAL formation in the UT/LS: 1) the source of aerosols from Africa and 2) the updraft mass flux from deep convective systems during the active phase of the South American monsoon system that transports aerosols to the UT/LS. Further satellite observations of aerosols and field campaigns are needed to provide useful information to find the origin and composition of the aerosols in the UT/LS during the South American monsoon.

Spatiotemporal and Vertical Distribution of Asian Tropopause Aerosol Layer Using Long-Term Multi-Source Data

The Asian tropopause aerosol layer (ATAL) is an enhanced aerosol concentration layer in the upper troposphere and lower stratosphere over Asia, and it has important effects on radiation balance, atmospheric circulation, regional climate, and atmospheric chemical processes. However, despite its importance, the specific structure and long-term variation trend of the ATAL have been rarely analyzed, which is critical for assessing the impact of ATAL on climate change and evaluating the performance of climate models. This study compared and analyzed the three-dimensional spatial distribution characteristics and temporal variability using CALIPSO, SAGEII, and MERRA-2 data and discussed the possible causes of the variation. The results showed that the ATAL began to appear in the mid-to-late 1990s and then strengthened rapidly until 2010, after which this trend was no longer observed. Moreover, significant heterogeneity existed in the distribution of aerosol concentration in the ATAL, showing north–south differences (NSDs) in both time and space. In addition, it was found that besides surface emissions, atmospheric circulation, the strength of convective transport, and stratosphere–troposphere exchange processes also contribute to this pattern. This study has important implications for quantifying the climate consequences of the ATAL.

Aerosol Effects on Clear‐Sky Shortwave Heating in the Asian Monsoon Tropopause Layer

AbstractThe Asian tropopause aerosol layer (ATAL) has emerged in recent decades with aerosol accumulation near tropopause above Asian Summer Monsoon region. Although ATAL effects on surface and top‐of‐atmosphere (TOA) radiation budgets are well established, the magnitude and variability of ATAL effects on radiative transfer within the tropopause layer remain poorly constrained. Here, we investigate the impacts of various aerosol types and layer structures on clear‐sky shortwave radiative heating in the Asian monsoon tropopause layer using reanalysis products and offline radiative transfer simulations. ATAL effects on shortwave radiative heating based on the Modern‐Era Retrospective Analysis for Research and Applications, version 2 aerosol reanalysis are on the order of 15% of mean clear‐sky radiative heating within the tropopause layer, although discrepancies among recent reanalysis and forecast products suggest that this ratio could be as small as ∼10% or as large as ∼70%. Uncertainties in surface and TOA flux effects are also large, with values spanning one order of magnitude at the TOA. ATAL effects on radiative heating peak between 150 and 80 hPa (360–400 K potential temperature) along the southern flank of the anticyclone. Clear‐sky and all‐sky shortwave heating are at local minima in this vertical range, which is situated between the positive influences of monsoon‐enhanced water vapor and the negative influence of the “ozone valley” in the monsoon lower stratosphere. ATAL effects also extend further toward the west, where diabatic vertical velocities remain upward despite descent in pressure coordinates.

Chemical analysis of the Asian tropopause aerosol layer (ATAL) with emphasis on secondary aerosol particles using aircraft-based in situ aerosol mass spectrometry

Abstract. Aircraft-borne in situ measurements of the chemical aerosol composition were conducted in the Asian tropopause aerosol layer (ATAL) over the Indian subcontinent in the summer of 2017, covering particle sizes below ∼3 µm. We have implemented a recently developed aerosol mass spectrometer, which adopts the laser desorption technique as well as the thermal desorption method for quantitative bulk information (i.e., a modified Aerodyne AMS), aboard the high-altitude research aircraft M-55 Geophysica. The instrument was deployed in July and August 2017 during the StratoClim EU campaign (Stratospheric and upper tropospheric processes for better Climate predictions) over Nepal, India, Bangladesh, and the Bay of Bengal, covering altitudes up to 20 kma.s.l. For particles with diameters between 10 nm and ∼3 µm, the vertical profiles of aerosol number densities from the eight research flights show significant enhancements in the altitude range of the ATAL. We observed enhancements in the mass concentrations of particulate nitrate, ammonium, and organics in a similar altitude range between approximately 13 and 18 km (corresponding to 360 and 410 K potential temperature). By means of the two aerosol mass spectrometry techniques, we show that the particles in the ATAL mainly consist of ammonium nitrate (AN) and organics. The single-particle analysis from laser desorption and ionization mass spectrometry revealed that a significant particle fraction (up to 70 % of all analyzed particles by number) within the ATAL results from the conversion of inorganic and organic gas-phase precursors, rather than from the uplift of primary particles from below. This can be inferred from the fact that the majority of the particles encountered in the ATAL consisted solely of secondary substances, namely an internal mixture of nitrate, ammonium, sulfate, and organic matter. These particles are externally mixed with particles containing primary components as well. The single-particle analysis suggests that the organic matter within the ATAL and in the lower stratosphere (even above 420 K) can partly be identified as organosulfates (OS), in particular glycolic acid sulfate, which are known as components indicative for secondary organic aerosol (SOA) formation. Additionally, the secondary particles are smaller in size compared to those containing primary components (mainly potassium, metals, and elemental carbon). The analysis of particulate organics with the thermal desorption method shows that the degree of oxidation for particles observed in the ATAL is consistent with expectations about secondary organics that were subject to photochemical processing and aging. We found that organic aerosol was less oxidized in lower regions of the ATAL (<380 K) compared to higher altitudes (here 390–420 K). These results suggest that particles formed in the lower ATAL are uplifted by prevailing diabatic heating processes and thereby subject to extensive oxidative aging. Thus, our observations are consistent with the concept of precursor gases being emitted from regional ground sources, subjected to rapid convective uplift, and followed by secondary particle formation and growth in the upper troposphere within the confinement of the Asian monsoon anticyclone (AMA). As a consequence, the chemical composition of these particles largely differs from the aerosol in the lower stratospheric background and the Junge layer.

The realization of autonomous, aircraft-based, real-time aerosol mass spectrometry in the upper troposphere and lower stratosphere

Abstract. We report on the developments that enabled the field deployment of a fully automated aerosol mass spectrometer, especially designed for high-altitude measurements on unpressurized aircraft. The merits of the two main categories of real-time aerosol mass spectrometry, i.e. (a) single-particle laser desorption and ionization and (b) continuous thermal desorption and electron impact ionization of aerosols, have been integrated into one compact apparatus with the aim to perform in situ real-time analysis of aerosol chemical composition. The demonstrated instrument, named the ERICA (European Research Council Instrument for Chemical composition of Aerosols), operated successfully aboard the high-altitude research aircraft M-55 Geophysica at altitudes up to 20 km while being exposed to ambient conditions of very low atmospheric pressure and temperature. A primary goal of those field deployments was the in situ study of the Asian tropopause aerosol layer (ATAL). During 11 research flights, the instrument operated for more than 49 h and collected chemical composition information of more than 150 000 single particles combined with quantitative chemical composition analysis of aerosol particle ensembles. This paper presents in detail the technical characteristics of the main constituent parts of the instrument, as well as the design considerations for its integration into the aircraft and its autonomous operation in the upper troposphere and lower stratosphere (UTLS). Additionally, system performance data from the first field deployments of the instrument are presented and discussed, together with exemplary mass spectrometry data collected during those flights.

Exploring the inorganic composition of the Asian Tropopause Aerosol Layer using medium-duration balloon flights

Abstract. Satellite observations have revealed an enhanced aerosol layer near the tropopause over Asia during the summer monsoon, called the “Asian Tropopause Aerosol Layer” (ATAL). In this work, aerosol particles in the ATAL were collected with a balloon-borne impactor near the tropopause region over India, using extended-duration balloon flights, in summer 2017 and winter 2018. The chemical composition of these particles was further investigated by quantitative analysis using offline ion chromatography. Nitrate (NO3-) and nitrite (NO2-) were found to be the dominant ions in the collected aerosols with values ranging between 87 and 343 ng m−3 at STP (standard temperature and pressure) during the summer campaign. In contrast, sulfate (SO42-) levels were found to be above the detection limit (>10 ng m−3 at STP) only in winter. In addition, we determined the origin of the air masses sampled during the flights using the analysis of back trajectories as well as a convective proxy from cloud-top temperature fields derived from a geostationary satellite. The results obtained from this analysis were put into the context of large-scale transport and aerosol distribution using GEOS-Chem chemical transport model simulations. The first flight in summer 2017 which sampled an air mass within the Asian monsoon anticyclone (AMA), influenced by convection over Western China, was associated with particle size diameters from 0.05 to 0.15 µm. In contrast, the second flight sampled air masses at the edge of the AMA associated with a larger particle size radius (>2 µm) with a higher NO2- concentration. The sampled air masses in winter 2018 were likely affected by smoke from the Pacific Northwest fire event in Canada, which occurred 7 months before our campaign, associated with concentration enhancements of SO42- and Ca2+. Overall, our results suggest that nitrogen-containing particles represent a large fraction of cloud-free and in-cloud aerosols populating the ATAL, which is partially in agreement with the results from aircraft measurements during the StratoClim (Stratospheric and upper tropospheric processes for better climate predictions) campaign. The exact nature of those particles is still unknown, but their coincidences with subvisible cirrus clouds and their sizes suggest nitric acid trihydrate (NAT) as a possible candidate, as NAT has already been observed in the tropical upper troposphere and lower stratosphere in other studies. Furthermore, GEOS-Chem model simulations indicate that lightning NOx emissions could have significantly impacted the production of nitrate aerosols sampled during the summer of 2017.

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

The Asian Tropopause Aerosol Layer (ATAL) is located in the Upper Troposphere and Lower Stratosphere (UTLS) during the Asian Summer Monsoon. However, what dynamical feature separates the ATAL from the well-known stratospheric ‘Junge layer’ is not yet clear. In this study, using the in-situ (Radiosonde, Ozonesonde, backscatter sonde and cryogenic frost-point hygrometer) observations from multiple locations in India (Gadanki (13.45° N, 79.18° E), Hyderabad (17.47° N, 78.58° E) and Varanasi (25.27° N, 82.99° E)) and multi-satellite observations ((Cloud-Aerosol Lidar and Infrared Pathfinder Observation, (CALIPSO), Atmospheric Chemistry Experiment (ACE) Fourier Transform Spectrometer (FTS) and Constellation Observation System for Meteorology, Ionosphere and Climate (COSMIC) Global Position System (GPS) Radio Occultation (RO) (COSMIC GPS-RO)) we show that the ATAL can exist up to the layer of maximum stability (LmaxS), located a few kilometers above the tropopause, determined using the square of Brunt Väisäla frequency. These in-situ observations over Indian stations collected during the ISRO-NASA Balloon Measurement Campaigns of the Asian Tropopause Aerosol Layer (BATAL) show that the ATAL top can reach up to ∼442 K potential temperature level over the Indian region. The LmaxS delineated from COSMIC GPSRO observations over the Asian Summer Monsoon Anticyclone (ASMA) region indicates that the top of ATAL can reach up to 454 K potential temperature level, which is lower than the earlier Lagrangian transport model predicted 460 K. The temperature inversion at LmaxS acts as a lid and constrains the direct transport of aerosols to higher altitudes.

The Asian tropopause aerosol layer within the 2017 monsoon anticyclone: microphysical properties derived from aircraft-borne in situ measurements

Abstract. The Asian summer monsoon is an effective pathway for aerosol particles and precursors from the planetary boundary layer over Central, South, and East Asia into the upper troposphere and lower stratosphere. An enhancement of aerosol particles within the Asian monsoon anticyclone (AMA), called the Asian tropopause aerosol layer (ATAL), has been observed by satellites. We discuss airborne in situ and remote sensing observations of aerosol microphysical properties conducted during the 2017 StratoClim field campaign within the AMA region. The aerosol particle measurements aboard the high-altitude research aircraft M55 Geophysica (maximum altitude reached of ∼20.5 km) were conducted with a modified ultra-high-sensitivity aerosol spectrometer – airborne (UHSAS-A; particle diameter detection range of 65 nm to 1 µm), the COndensation PArticle counting System (COPAS, detecting total concentrations of submicrometer-sized particles), and the New Ice eXpEriment – Cloud and Aerosol Spectrometer with Detection of POLarization (NIXE-CAS-DPOL). In the COPAS and UHSAS-A vertical particle mixing ratio (PMR) profiles and the size distribution profiles (for number, surface area, and volume concentration), the ATAL is evident as a distinct layer between ∼370 and 420 K potential temperature (Θ). Within the ATAL, the maximum detected PMRs (from the median profiles) were ∼700 mg−1 for particle diameters between 65 nm and 1 µm (UHSAS-A) and higher than 2500 mg−1 for diameters larger than 10 nm (COPAS). These values are up to 2 times higher than those previously found at similar altitudes in other tropical locations. The difference between the PMR profiles measured by the UHSAS-A and the COPAS indicate that the region below the ATAL at Θ levels from 350 to 370 K is influenced by the nucleation of aerosol particles (diameter <65 nm). We provide detailed analyses of the vertical distribution of the aerosol particle size distributions and the PMR and compare these with previous tropical and extratropical measurements. The backscatter ratio (BR) was calculated based on the aerosol particle size distributions measured in situ. The resulting data set was compared with the vertical profiles of the BR detected by the multiwavelength aerosol scatterometer (MAS) and an airborne miniature aerosol lidar (MAL) aboard the M55 Geophysica and by the satellite-borne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP). The data of all four methods largely agree with one another, showing enhanced BR values in the altitude range of the ATAL (between ∼15 and 18.5 km) with a maximum at 17.5 km altitude. By means of the AMA-centered equivalent latitude calculated from meteorological reanalysis data, it is shown that such enhanced values of the BR larger than 1.1 could only be observed within the confinement of the AMA.

In situ observation of new particle formation (NPF) in the tropical tropopause layer of the 2017 Asian monsoon anticyclone – Part 1: Summary of StratoClim results

Abstract. During the monsoon season of the year 2017 the airborne StratoClim mission took place in Kathmandu, Nepal, with eight mission flights of the M-55 Geophysica in the upper troposphere–lower stratosphere (UTLS) of the Asian monsoon anticyclone (AMA) over northern India, Nepal, and Bangladesh. More than 100 events of new particle formation (NPF) were observed. In total, more than 2 h of flight time was spent under NPF conditions as indicated by the abundant presence of nucleation-mode aerosols, i.e. with particle diameters dp smaller than 15 nm, which were detected in situ by means of condensation nuclei counting techniques. Mixing ratios of nucleation-mode particles (nnm) of up to ∼ 50 000 mg−1 were measured at heights of 15–16 km (θ ≈ 370 K). NPF was most frequently observed at ∼ 12–16 km altitude (θ ≈ 355–380 K) and mainly below the tropopause. Resulting nnm remained elevated (∼ 300–2000 mg−1) up to altitudes of ∼ 17.5 km (θ ≈ 400 K), while under NPF conditions the fraction (f) of sub-micrometre-sized non-volatile residues (dp > 10 nm) remained below 50 %. At ∼ 12–14 km (θ ≈ 355–365 K) the minimum of f (< 15 %) was found, and underneath, the median f generally remains below 25 %. The persistence of particles at nucleation-mode sizes is limited to a few hours, mainly due to coagulation, as demonstrated by a numerical simulation. The frequency of NPF events observed during StratoClim 2017 underlines the importance of the AMA as a source region for UTLS aerosols and for the formation and maintenance of the Asian tropopause aerosol layer (ATAL). The observed abundance of NPF-produced nucleation-mode particles within the AMA is not unambiguously attributable to (a) specific source regions in the boundary layer (according to backward trajectory analyses), or (b) the direct supply with precursor material by convective updraught (from correlations of NPF with carbon monoxide), or (c) the recent release of NPF-capable material from the convective outflow (according to air mass transport times in the tropical tropopause layer, TTL). Temperature anomalies with ΔT of 2 K (peak-to-peak amplitude), as observed at a horizontal wavelength of ∼ 70–100 km during a level flight of several hours, match with NPF detections and represent an additional mechanism for local increases in supersaturation of the NPF precursors. Effective precursor supply and widely distributed temperature anomalies within the AMA can explain the higher frequency of intense NPF observed during StratoClim 2017 than all previous NPF detections with COPAS (COndensation PArticle counting System) at TTL levels over Brazil, northern Australia, or West Africa.

High-resolution optical constants of crystalline ammonium nitrate for infrared remote sensing of the Asian Tropopause Aerosol Layer

Abstract. Infrared spectroscopic observations have shown that crystalline ammonium nitrate (AN) particles are an abundant constituent of the upper tropospheric aerosol layer which is formed during the Asian summer monsoon period, the so-called Asian Tropopause Aerosol Layer (ATAL). At upper tropospheric temperatures, the thermodynamically stable phase of AN is different from that at 298 K, meaning that presently available room-temperature optical constants of AN, that is, the real and imaginary parts of the complex refractive index, cannot be applied for the quantitative analysis of these infrared measurements. In this work, we have retrieved the first low-temperature data set of optical constants for crystalline AN in the 800–6000 cm−1 wavenumber range with a spectral resolution of 0.5 cm−1. The optical constants were iteratively derived from an infrared extinction spectrum of 1 µm sized AN particles suspended in a cloud chamber at 223 K. The uncertainties of the new data set were carefully assessed in a comprehensive sensitivity analysis. We show that our data accurately fit aircraft-borne infrared measurements of ammonium nitrate particles in the ATAL.

Convective uplift of pollution from the Sichuan Basin into the Asian monsoon anticyclone during the StratoClim aircraft campaign

Abstract. 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 intense convective activity over South China and Sichuan. Comparisons between brightness temperatures (BTs) at 10.8 µm 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. A comparison between CO and O3 concentrations from Meso-NH and airborne observations (StratoClim and IAGOS (In-service Aircraft for a Global Observing System)) 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 the resolution is too coarse, 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. It is noteworthy that 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 in CO concentration over the 10–20 km range that lasted about 2 d. The impact of pollution uplift from three regions (India, China, and Sichuan) averaged over the first 10 d 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 concentration in the 10–15 km layer. Moreover, during this period a large part (35 %) of the Chinese contribution comes from the Sichuan Basin alone.

Lower-stratospheric aerosol measurements in eastward-shedding vortices over Japan from the Asian summer monsoon anticyclone during the summer of 2018

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.

Global modeling studies of composition and decadal trends of the Asian Tropopause Aerosol Layer

Abstract. 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). Due to the dynamical variability of the AMA, the dearth of in situ observations in this region, the complexity of the emission sources and of transport pathways, knowledge of the ATAL properties in terms of aerosol budget, chemical composition, as well as its variability and temporal trend is still largely uncertain. 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 typical “double-peak” vertical profile of aerosols for the ATAL. We attribute the upper peak (around 100 hPa, predominant during early ATAL, e.g., in June) to dry aerosols, possibly from nucleation processes, and the lower peak (around 250 hPa, predominant for a well-developed and late ATAL, e.g., in July and August) to cloud-borne aerosols associated with convective clouds. We find that mineral dust (present in both peaks) is the dominant aerosol by mass in the ATAL, showing a large interannual variability but no long-term trend, due to its natural variability. The results between 120 and 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. Nitrate aerosols are not considered in MAM7. The analysis of the anthropogenic and biomass burning aerosols shows a positive trend for all aerosols simulated by CESM-MAM7.

Vertical and spatial distribution of elevated aerosol layers obtained using long-term ground-based and space-borne lidar observations

In this study, long-term ground-based and space-borne lidar measurements are used to understand the vertical (surface to 30 km) and spatial distribution of aerosols. First, the vertical distribution of aerosol extinction (AE) covering from near surface to 30 km is provided by combining Micro Pulse Lidar and Mie lidar observations co-located over a tropical station Gadanki (13.5oN, 79.2oE), India. The presence of two elevated aerosol layers, one between 2 and 5 km (lower troposphere) and the other between 15 and 18 km (Upper Troposphere and Lower Stratosphere (UTLS)), are simultaneously observed during the Indian summer monsoon season. Second, the spatial extent of these elevated aerosol layers obtained using Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) measurements reveals the presence of the lower layer extending from Africa to South Asia during both pre–monsoon and monsoon seasons. However, the UTLS layer is confined from middle-east to the China Sea only during monsoon season, also known as Asian Tropopause Aerosol Layer (ATAL). Third, aerosol sub-types obtained for these elevated aerosol layers using CALIPSO measurements reveals the dominance of polluted dust (44.6%) whereas the occurrence frequency of polluted continental, dust and elevated smoke is ~19.6%, 20.7% and 13.1%, respectively, for the lower layer. However, the frequency of volcanic ash and sulfate aerosols is ~50.3% and 49.7%, respectively, for the UTLS layer. Depolarization ratio (color ratio) values varies between 0.21 and 0.34 (>0.6) in the lower layer while the values >0.15 (<0.6) are present in the UTLS layer during monsoon season revealing the influence of non-spherical and coarse mode particles in the lower layer while spherical and fine mode particles in the UTLS region over the site. This information is very much useful in estimating reliable radiative forcing due to these elevated aerosol layers on the background atmosphere involved in assessing their impact on the regional climate.

Formation and dissipation dynamics of the Asian tropopause aerosol layer

The Asian tropopause aerosol layer (ATAL) is characterized by enhanced aerosol concentrations in the Asian summer monsoon anticyclone in the upper troposphere and lower stratosphere at 13–18 km altitude. A growing body of evidence suggests that the aerosol enhancement is closely connected with deep convection during the monsoon. However, the origin of the aerosols is under debate, and the key factors that determine the ATAL variability remain poorly understood. We investigated the formation and dissipation mechanisms of the ATAL and the inter-annual variation from a dynamical viewpoint using satellite observations and meteorological reanalysis data from 2012 to 2018. We identified the northern Bay of Bengal and adjacent land area, where air pollution from the Indian subcontinent converges, as the major convection source area of aerosols to the ATAL. The spatial extent of the ATAL, represented by the mean attenuated scattering ratio from satellite measurements, appears to be related to a secondary circulation driven by the stratospheric quasi-biennial oscillation. The aerosols are not homogeneously distributed within the ATAL, and descending motion in the western part is found to play an important role in dissipation of the layer. These findings elucidate the ATAL dynamics and associated regional and global air pollution transports.

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.

Aerosol variations in the upper troposphere and lower stratosphere over the Tibetan Plateau

Satellite measurements and model simulations indicate the existence of the Asian tropopause aerosol layer (ATAL)—an enhanced aerosol layer in the upper troposphere and lower stratosphere (UTLS) associated with the Asian summer monsoon (ASM)—although it has rarely been evidenced by snapshots of balloon-borne in situ measurements. To better understand how the ATAL evolves, a portable optical particle counter (POPS) onboard a stratospheric balloon was released over the Tibetan Plateau (TP) during the ASM period of 2019. The POPS detected the ATAL in the UTLS during the ascending, descending periods, as well as during its quasi-horizontal floating periods. The aerosol number density in the ATAL showed obvious vertical variability. The peak aerosol number density in the ATAL was 180 cm−3 around the tropopause during the ascending and descending period and the maximum aerosol number density was 290 cm−3 around the tropopause during the floating period. And the aerosol concentration observed over the TP in the 2019 summer was approximately five times larger than that in the 2018 summer. Lagrangian simulations reveal that the minority of the observed aerosol particles were directly elevated in a region of uplift south of the Himalayas, and the majority of the particles were transported from the UTLS region situated approximately between the isentropic surfaces of 370 and 460 K. Up to 14% of the observed aerosol particles were directly influenced by the volcanic plumes from the eruption of the volcano Raikoke in June 2019.