Satellite observations have shown that the Asian Summer Monsoon strongly influences the upper troposphere and lower stratosphere (UTLS) aerosol morphology through its role in the formation of the ...Asian Tropopause Aerosol Layer (ATAL). Stratospheric Aerosol and Gas Experiment II solar occultation and Cloud‐Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) lidar observations show that summertime UTLS Aerosol Optical Depth (AOD) between 13 and 18 km over Asia has increased by three times since the late 1990s. Here we present the first in situ balloon measurements of aerosol backscatter in the UTLS from Western China, which confirm high aerosol levels observed by CALIPSO since 2006. Aircraft in situ measurements suggest that aerosols at lower altitudes of the ATAL are largely composed of carbonaceous and sulfate materials (carbon/sulfur elemental ratio ranging from 2 to 10). Back trajectory analysis from Cloud‐Aerosol Lidar with Orthogonal Polarization observations indicates that deep convection over the Indian subcontinent supplies the ATAL through the transport of pollution into the UTLS. Time series of deep convection occurrence, carbon monoxide, aerosol, temperature, and relative humidity suggest that secondary aerosol formation and growth in a cold, moist convective environment could play an important role in the formation of ATAL. Finally, radiative calculations show that the ATAL layer has exerted a short‐term regional forcing at the top of the atmosphere of −0.1 W/m2 in the past 18 years.
Key Points
Increase of summertime upper tropospheric aerosol levels over Asia since the 1990s
Upper tropospheric enhancement also observed by in situ backscatter measurements
Significant regional radiative forcing of −0.1 W/m2
Advanced measurement and modelling techniques are employed to estimate the partitioning of atmospheric water between the gas phase and the condensed phase in and around cirrus clouds, and thus to ...identify in-cloud and out-of-cloud supersaturations with respect to ice. In November 2008 the newly developed balloon-borne backscatter sonde COBALD (Compact Optical Backscatter and AerosoL Detector) was flown 14 times together with a CFH (Cryogenic Frost point Hygrometer) from Lindenberg, Germany (52° N, 14° E). The case discussed here in detail shows two cirrus layers with in-cloud relative humidities with respect to ice between 50% and 130%. Global operational analysis data of ECMWF (roughly 1° × 1° horizontal and 1 km vertical resolution, 6-hourly stored fields) fail to represent ice water contents and relative humidities. Conversely, regional COSMO-7 forecasts (6.6 km × 6.6 km, 5-min stored fields) capture the measured humidities and cloud positions remarkably well. The main difference between ECMWF and COSMO data is the resolution of small-scale vertical features responsible for cirrus formation. Nevertheless, ice water contents in COSMO-7 are still off by factors 2–10, likely reflecting limitations in COSMO's ice phase bulk scheme. Significant improvements can be achieved by comprehensive size-resolved microphysical and optical modelling along backward trajectories based on COSMO-7 wind and temperature fields, which allow accurate computation of humidities, homogeneous ice nucleation, resulting ice particle size distributions and backscatter ratios at the COBALD wavelengths. However, only by superimposing small-scale temperature fluctuations, which remain unresolved by the numerical weather prediction models, can we obtain a satisfying agreement with the observations and reconcile the measured in-cloud non-equilibrium humidities with conventional ice cloud microphysics. Conversely, the model-data comparison provides no evidence that additional changes to ice-cloud microphysics – such as heterogeneous nucleation or changing the water vapour accommodation coefficient on ice – are required.
This paper presents results of the extensive field campaign CLACE 2010 (Cloud and Aerosol Characterization Experiment) performed in summer 2010 at the Jungfraujoch (JFJ) and the Kleine Scheidegg ...(KLS) in the Swiss Alps. The main goal of this campaign was to investigate the vertical variability of aerosol optical properties around the JFJ and to show the consistency of the different employed measurement techniques considering explicitly the effects of relative humidity (RH) on the aerosol light scattering. Various aerosol optical and microphysical parameters were recorded using in-situ and remote sensing techniques. In-situ measurements of aerosol size distribution, light scattering, light absorption and scattering enhancement due to water uptake were performed at the JFJ at 3580 m a.s.l.. A unique set-up allowed remote sensing measurements of aerosol columnar and vertical properties from the KLS located about 1500 m below and within the line of sight to the JFJ (horizontal distance of approx. 4.5 km). In addition, two satellite retrievals from the Spinning Enhanced Visible and Infrared Imager (SEVIRI) and the Moderate Resolution Imaging Spectroradiometer (MODIS) as well as back trajectory analyses were added to the comparison to account for a wider geographical context. All in-situ and remote sensing measurements were in clear correspondence. The ambient extinction coefficient measured in situ at the JFJ agreed well with the KLS-based LIDAR (Light Detection and Ranging) retrieval at the altitude-level of the JFJ under plausible assumptions on the LIDAR ratio. However, we can show that the quality of this comparison is affected by orographic effects due to the exposed location of the JFJ on a saddle between two mountains and next to a large glacier. The local RH around the JFJ was often higher than in the optical path of the LIDAR measurement, especially when the wind originated from the south via the glacier, leading to orographic clouds which remained lower than the LIDAR beam. Furthermore, the dominance of long-range transported Saharan dust was observed in all measurements for several days, however only for a shorter time period in the in-situ measurements due to the vertical structure of the dust plume. The optical properties of the aerosol column retrieved from SEVIRI and MODIS showed the same magnitude and a similar temporal evolution as the measurements at the KLS and the JFJ. Remaining differences are attributed to the complex terrain and simplifications in the aerosol retrieval scheme in general.
The AquaVIT-1 intercomparison of atmospheric water vapor measurement techniques was conducted at the aerosol and cloud simulation chamber AIDA (Aerosol Interaction and Dynamics in the Atmosphere) at ...the Karlsruhe Institute of Technology, Germany, in October 2007. The overall objective was to intercompare state-of-the-art and prototype atmospheric hygrometers with each other and with independent humidity standards under controlled conditions. This activity was conducted as a blind intercomparison with coordination by selected referees. The effort was motivated by persistent discrepancies found in atmospheric measurements involving multiple instruments operating on research aircraft and balloon platforms, particularly in the upper troposphere and lower stratosphere, where water vapor reaches its lowest atmospheric values (less than 10 ppm). With the AIDA chamber volume of 84 m3, multiple instruments analyzed air with a common water vapor mixing ratio, by extracting air into instrument flow systems, by locating instruments inside the chamber, or by sampling the chamber volume optically. The intercomparison was successfully conducted over 10 days during which pressure, temperature, and mixing ratio were systematically varied (50 to 500 hPa, 185 to 243 K, and 0.3 to 152 ppm). In the absence of an accepted reference instrument, the absolute accuracy of the instruments was not established. To evaluate the intercomparison, the reference value was taken to be the ensemble mean of a core subset of the measurements. For these core instruments, the agreement between 10 and 150 ppm of water vapor is considered good with variation about the reference value of about ±10% (±1σ). In the region of most interest between 1 and 10 ppm, the core subset agreement is fair with variation about the reference value of ±20% (±1σ). The upper limit of precision was also derived for each instrument from the reported data. The implication for atmospheric measurements is that the substantially larger differences observed during in-flight intercomparisons stem from other factors associated with the moving platforms or the non-laboratory environment. The success of AquaVIT-1 provides a template for future intercomparison efforts with water vapor or other species that are focused on improving the analytical quality of atmospheric measurements on moving platforms.
A nascent in situ cirrus was observed on January 11, 2019 in the tropical tropopause layer (TTL) over the southwestern Indian Ocean, with the use of balloon‐borne instruments. Data from cryogenic ...frost point hygrometer (CFH) and Compact Optical Backscatter and AerosoL Detector (COBALD) instruments were used to characterize the cirrus and its environment. Optical modeling was employed to estimate the cirrus microphysical properties from the COBALD backscatter measurements. Newly fomed ice crystals with radius <1 μm and concentration ∼500 L−1 were reported at the tropopause. The relatively low concentration and CFH ice supersaturation (1.5) suggests a homogeneous freezing event stalled by a high‐frequency gravity wave. The observed vertical wind speed and temperature anomalies that triggered the cirrus formation were due to a 1.5‐km vertical‐scale wave, as shown by a spectral analysis. This cirrus observation shortly after nucleation is beyond remote sensing capabilities and presents a type of cirrus never reported before.
Plain Language Summary
Ice clouds are very common in the tropical tropopause layer, a layer of the atmosphere between 14 and 18 km separating the troposphere and the stratosphere. Ice clouds can be formed in situ, generated by cold temperature anomalies due to atmospheric disturbances. In this observational study, we use data from instruments that were flown on the same balloon on January 11, 2019 from Réunion Island, in the southwestern Indian Ocean. We report an ice cloud at the tropopause, at ∼16.5 km, composed of ice particles with a concentration of more than 500 per liter. This suggests that the ice cloud formed by homogeneous freezing, that is, the freezing of airborne aqueous solutions. In addition, an abrupt increase in ascent rate of the balloon is related to an atmospheric disturbance which cooled the air and possibly led to the ice cloud formation. The tiny size of the ice crystals indicates that they have just formed. This is a very rare observation because nucleation events are very short.
Key Points
First in situ observation of a nascent tropical tropopause cirrus
Homogeneous formation of tiny ice crystals (<1 μm) is due to a short vertical scale gravity wave at the tropopause
Such optically thin cirrus clouds would be missed by current aircraft instruments/remote sensing systems
The Asian summer monsoon anticyclone (ASMA) is a major
meteorological system of the upper troposphere–lower stratosphere (UTLS)
during boreal summer. It is known to contain enhanced tropospheric ...trace
gases and aerosols, due to rapid lifting from the boundary layer by deep
convection and subsequent horizontal confinement. Given its dynamical
structure, the ASMA represents an efficient pathway for the transport of
pollutants to the global stratosphere. A detailed understanding of the thermal
structure and processes in the ASMA requires accurate in situ measurements.
Within the StratoClim project we performed state-of-the-art balloon-borne
measurements of temperature, water vapor, ozone and aerosol backscatter from
two stations on the southern slopes of the Himalayas. In total, 63 balloon
soundings were conducted during two extensive monsoon-season campaigns, in
August 2016 in Nainital, India (29.4∘ N, 79.5∘ E), and in
July–August 2017 in Dhulikhel, Nepal (27.6∘ N, 85.5∘ E);
one shorter post-monsoon campaign was also carried out in November 2016 in Nainital. These
measurements provide unprecedented insights into the UTLS thermal structure,
the vertical distributions of water vapor, ozone and aerosols, cirrus cloud
properties and interannual variability in the ASMA. Here we provide an overview
of all of the data collected during the three campaign periods, with focus on
the UTLS region and the monsoon season. We analyze the vertical structure of
the ASMA in terms of significant levels and layers, identified from the
temperature and potential temperature lapse rates and Lagrangian backward
trajectories, which provides a framework for relating the measurements to local
thermodynamic properties and the large-scale anticyclonic flow. Both the
monsoon-season campaigns show evidence of deep convection and confinement
extending up to 1.5–2 km above the cold-point tropopause (CPT), yielding a
body of air with high water vapor and low ozone which is prone to being lifted
further and mixed into the free stratosphere. Enhanced aerosol backscatter
also reveals the signature of the Asian tropopause aerosol layer (ATAL) over
the same region of altitudes. The Dhulikhel 2017 campaign was characterized
by a 5 K colder CPT on average than in Nainital 2016 and a local water
vapor maximum in the confined lower stratosphere, about 1 km above the CPT.
Data assessment and modeling studies are currently ongoing with the aim of
fully exploring this dataset and its implications with respect to stratospheric
moistening via the ASMA system and related processes.
Observations of high supersaturations with respect to ice inside cirrus clouds with high ice water content (> 0.01 g kg−1) and high crystal number densities (> 1 cm−3) are challenging our ...understanding of cloud microphysics and of climate feedback processes in the upper troposphere. However, single measurements of a cloudy air mass provide only a snapshot from which the persistence of ice supersaturation cannot be judged. We introduce here the "cirrus match technique" to obtain information about the evolution of clouds and their saturation ratio. The aim of these coordinated balloon soundings is to analyze the same air mass twice. To this end the standard radiosonde equipment is complemented by a frost point hygrometer, "SnowWhite", and a particle backscatter detector, "COBALD" (Compact Optical Backscatter AerosoL Detector). Extensive trajectory calculations based on regional weather model COSMO (Consortium for Small-Scale Modeling) forecasts are performed for flight planning, and COSMO analyses are used as a basis for comprehensive microphysical box modeling (with grid scale of 2 and 7 km, respectively). Here we present the results of matching a cirrus cloud to within 2–15 km, realized on 8 June 2010 over Payerne, Switzerland, and a location 120 km downstream close to Zurich. A thick cirrus cloud was detected over both measurement sites. We show that in order to quantitatively reproduce the measured particle backscatter ratios, the small-scale temperature fluctuations not resolved by COSMO must be superimposed on the trajectories. The stochastic nature of the fluctuations is captured by ensemble calculations. Possibilities for further improvements in the agreement with the measured backscatter data are investigated by assuming a very slow mass accommodation of water on ice, the presence of heterogeneous ice nuclei, or a wide span of (spheroidal) particle shapes. However, the resulting improvements from these microphysical refinements are moderate and comparable in magnitude with changes caused by assuming different regimes of temperature fluctuations for clear-sky or cloudy-sky conditions, highlighting the importance of proper treatment of subscale fluctuations. The model yields good agreement with the measured backscatter over both sites and reproduces the measured saturation ratios with respect to ice over Payerne. Conversely, the 30% in-cloud supersaturation measured in a massive 4 km thick cloud layer over Zurich cannot be reproduced, irrespective of the choice of meteorological or microphysical model parameters. The measured supersaturation can only be explained by either resorting to an unknown physical process, which prevents the ice particles from consuming the excess humidity, or – much more likely – by a measurement error, such as a contamination of the sensor housing of the SnowWhite hygrometer by a precipitation drop from a mixed-phase cloud just below the cirrus layer or from some very slight rain in the boundary layer. This uncertainty calls for in-flight checks or calibrations of hygrometers under the special humidity conditions in the upper troposphere.
The volcanic aerosol plume resulting from the Eyjafjallajökull eruption in Iceland in April and May 2010 was detected in clear layers above Switzerland during two periods (17–19 April 2010 and 16–19 ...May 2010). In-situ measurements of the airborne volcanic plume were performed both within ground-based monitoring networks and with a research aircraft up to an altitude of 6000 m a.s.l. The wide range of aerosol and gas phase parameters studied at the high altitude research station Jungfraujoch (3580 m a.s.l.) allowed for an in-depth characterization of the detected volcanic aerosol. Both the data from the Jungfraujoch and the aircraft vertical profiles showed a consistent volcanic ash mode in the aerosol volume size distribution with a mean optical diameter around 3 ± 0.3 μm. These particles were found to have an average chemical composition very similar to the trachyandesite-like composition of rock samples collected near the volcano. Furthermore, chemical processing of volcanic sulfur dioxide into sulfate clearly contributed to the accumulation mode of the aerosol at the Jungfraujoch. The combination of these in-situ data and plume dispersion modeling results showed that a significant portion of the first volcanic aerosol plume reaching Switzerland on 17 April 2010 did not reach the Jungfraujoch directly, but was first dispersed and diluted in the planetary boundary layer. The maximum PM10 mass concentrations at the Jungfraujoch reached 30 μgm−3 and 70 μgm−3 (for 10-min mean values) duri ng the April and May episode, respectively. Even low-altitude monitoring stations registered up to 45 μgm−3 of volcanic ash related PM10 (Basel, Northwestern Switzerland, 18/19 April 2010). The flights with the research aircraft on 17 April 2010 showed one order of magnitude higher number concentrations over the northern Swiss plateau compared to the Jungfraujoch, and a mass concentration of 320 (200–520) μgm−3 on 18 May 2010 over the northwestern Swiss plateau. The presented data significantly contributed to the time-critical assessment of the local ash layer properties during the initial eruption phase. Furthermore, dispersion models benefited from the detailed information on the volcanic aerosol size distribution and its chemical composition.
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.
We present high-resolution measurements of water vapour, aerosols and clouds in the Arctic stratosphere in January and February 2010 carried out by in situ instrumentation on balloon sondes and ...high-altitude aircraft combined with satellite observations. The measurements provide unparalleled evidence of dehydration and rehydration due to gravitational settling of ice particles. An extreme cooling of the Arctic stratospheric vortex during the second half of January 2010 resulted in a rare synoptic-scale outbreak of ice polar stratospheric clouds (PSCs) remotely detected by the lidar aboard the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) satellite. The widespread occurrence of ice clouds was followed by sedimentation and consequent sublimation of ice particles, leading to vertical redistribution of water inside the vortex. A sequence of balloon and aircraft soundings with chilled mirror and Lyman- α hygrometers (Cryogenic Frostpoint Hygrometer, CFH; Fast In Situ Stratospheric Hygrometer, FISH; Fluorescent Airborne Stratospheric Hygrometer, FLASH) and backscatter sondes (Compact Optical Backscatter Aerosol Detector, COBALD) conducted in January 2010 within the LAPBIAT (Lapland Atmosphere-Biosphere Facility) and RECONCILE (Reconciliation of Essential Process Parameters for an Enhanced Predictability of Arctic Stratospheric Ozone Loss and its Climate Interactions) campaigns captured various phases of this phenomenon: ice formation, irreversible dehydration and rehydration. Consistent observations of water vapour by these independent measurement techniques show clear signatures of irreversible dehydration of the vortex air by up to 1.6 ppmv in the 20–24 km altitude range and rehydration by up to 0.9 ppmv in a 1 km thick layer below. Comparison with space-borne Aura MLS (Microwave Limb Sounder) water vapour observations allow the spatiotemporal evolution of dehydrated air masses within the Arctic vortex to be derived and upscaled.
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