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Despite their proven importance for the atmospheric radiative energy budget, the effect of cirrus on climate and the magnitude of their modification by human activity is not well quantified. Besides anthropogenic pollution sources on the ground, aviation has a large local effect on cirrus microphysical and radiative properties via the formation of contrails and their transition to contrail cirrus. To investigate the anthropogenic influence on natural cirrus, we compare the microphysical properties of cirrus measured at mid-latitude (ML) regions (<60 ∘ N) that are often affected by aviation and pollution with cirrus measured in the same season in comparatively pristine high latitudes (HLs; ≥60 ∘ N). The number concentration, effective diameter, and ice water content of the observed cirrus are derived from in situ measurements covering ice crystal sizes between 2 and 6400 µm collected during the CIRRUS-HL campaign (Cirrus in High Latitudes) in June and July 2021. We analyse the dependence of cirrus microphysical properties on altitude and latitude and demonstrate that the median ice number concentration is an order of magnitude larger in the measured mid-latitude cirrus, with 0.0086 cm-3 , compared to the high-latitude cirrus, with 0.001 cm-3. Ice crystals in mid-latitude cirrus are on average smaller than in high-latitude cirrus, with a median effective diameter of 165 µm compared to 210 µm , and the median ice water content in mid-latitude cirrus is higher (0.0033 gm-3) than in high-latitude cirrus (0.0019 gm-3). In order to investigate the cirrus properties in relation to the region of formation, we combine the airborne observations with 10 d backward trajectories to identify the location of cirrus formation and the cirrus type, i.e. in situ or liquid origin cirrus, depending on whether there is only ice or also liquid water present in the cirrus history, respectively. The cirrus formed and measured at mid-latitudes (M–M) have a particularly high ice number concentration and low effective diameter. This is very likely a signature of contrails and contrail cirrus, which is often observed in the in situ origin cirrus type. In contrast, the largest effective diameter and lowest number concentration were found in the cirrus formed and measured at high latitudes (H–H) along with the highest relative humidity over ice (RHi). On average, in-cloud RHi was above saturation in all cirrus. While most of the H–H cirrus were of an in situ origin, the cirrus formed at mid-latitudes and measured at high latitudes (M–H) were mainly of liquid origin. A pristine Arctic background atmosphere with relatively low ice nuclei availability and the extended growth of few nucleated ice crystals may explain the observed RHi and size distributions. The M–H cirrus are a mixture of the properties of M–M and H–H cirrus (preserving some of the initial properties acquired at mid-latitudes and transforming under Arctic atmospheric conditions). Our analyses indicate that part of the cirrus found at high latitudes is actually formed at mid-latitudes and therefore affected by mid-latitude air masses, which have a greater anthropogenic influence. [ABSTRACT FROM AUTHOR]

During the StratoClim Geophysica campaign, air with total water mixing ratios up to 200 ppmv and ozone up to 250 ppbv was observed within the Asian summer monsoon anticyclone up to 1.7 km above the local cold-point tropopause (CPT). To investigate the temporal evolution of enhanced water vapor being transported into the stratosphere, we conduct forward trajectory simulations using both a microphysical and an idealized freeze-drying model. The models are initialized at the measurement locations and the evolution of water vapor and ice is compared with satellite observations of MLS and CALIPSO. Our results show that these extremely high water vapor values observed above the CPT are very likely to undergo significant further freeze-drying due to experiencing extremely cold temperatures while circulating in the anticyclonic "dehydration carousel". We also use the Lagrangian dry point (LDP) of the merged back-and-forward trajectories to reconstruct the water vapor fields. The results show that the extremely high water vapor mixed with the stratospheric air has a negligible impact on the overall water vapor budget. The LDP mixing ratios are a better proxy for the large-scale water vapor distributions in the stratosphere during this period. [ABSTRACT FROM AUTHOR]

Cirrus clouds that form in the tropical tropopause layer (TTL) can play a key role in vertical transport through the upper troposphere and lower stratosphere, which can significantly impact the radiative energy budget and stratospheric chemistry. The main scientific objectives of this work are to (a) investigate the influence of predefined versus non-predefined categories of ice hydrometeors and ice habit on convectively driven TTL cirrus in simulations of the Asian summer monsoon, and (b) determine the optimal model configuration to adequately simulate TTL cirrus clouds. During the StratoClim field campaign in 2017, aircraft measurements from the southern slopes of the Himalayas captured high ice water content (HIWC) up to 2400 ppmv and ice particle aggregates exceeding 700 µm in size with unusually long residence times. The observed ice particles were mainly of liquid origin, with a small amount formed in situ. The corresponding profile of IWC from the ERA5 reanalysis corroborates the presence of HIWC detrained from deep convective plumes in the TTL but underestimates HIWC by an order of magnitude. We compare the aircraft measurements to a set of numerical experiments at the scales of large-eddy simulations (LES) of the same case study that employ different microphysics schemes. In the TTL, only the scheme that predicts ice habits can reproduce the observed HIWC, ice number concentration, and bimodal ice particle size distribution. The lower range of particle sizes is mostly represented by planar and columnar habits, while the upper range is dominated by aggregates. Large aggregates with sizes between 600 and 800 µm have fall speeds of less than 20 cm s-1, which explains the long residence time of the aggregates in the TTL. Planar ice particles of liquid origin contribute substantially to HIWC. The columnar and aggregates habits are in the in-situ range with lower IWC and number concentration. For all habits, the ice number concentration increases with decreasing temperature. For the planar ice habit, relative humidity is inversely correlated with fall speed. This correlation is less evident for the other two ice habits. In the lower range of supersaturation with respect to ice, columnar habit has the highest fall speed. The difference in ice number concentration across habits can be up to four orders of magnitude, and aggregates occurring in much smaller numbers. We demonstrate and quantify the linear relationship between the differential sedimentation of pristine ice crystals and the size of the aggregates that form when pristine crystals collide. The slope of this relationship depends on which pristine ice habit sediments faster. Each simulated ice habit is associated with distinct radiative and latent heating rates. This study suggests that a model configuration nested down to LES scales with a microphysical parameterization that predicts ice shape evolution is crucial to provide an accurate representation of the microphysical properties of TTL cirrus, and thus the associated (de)hydration process. [ABSTRACT FROM AUTHOR]

During winter 2015/2016 the Arctic stratosphere was characterized by extraordinarily low temperatures in connection with the occurrence of extensive polar stratospheric clouds. From mid of December 2015 until mid of March 2016 the German research aircraft HALO (High Altitude and Long-Range Research Aircraft) was deployed to probe the lowermost stratosphere in the Arctic region within the POLSTRACC (Polar Stratosphere in a Changing Climate) mission. More than twenty flights have been conducted out of Kiruna/Sweden and Oberpfaffenhofen/Germany, covering the whole winter period. Besides total reactive nitrogen (NOy), observations of nitrous oxide, nitric acid, ozone and water were used for this study. Total reactive nitrogen and its partitioning between gas- and particle phase are key parameters for understanding processes controlling the ozone budget in the polar winter stratosphere. The redistribution of total reactive nitrogen was evaluated by using tracer-tracer correlations. In January air masses with extensive nitrification were encountered at altitudes between 12 and 15 km. The excess NOy amounted up to about 6 ppb. During several flights, along with gas-phase nitrification, indications for extensive occurrence of nitric acid containing particles at flight altitude were found. These observations support the assumption of sedimentation and subsequent evaporation of nitric acid containing particles leading to redistribution of total reactive nitrogen. Remnants of nitrified air masses have been observed until mid of March. Between end of February and mid of March also de-nitrified air masses have been observed in connection with high potential temperatures. Using tracer-tracer correlations, missing total reactive nitrogen was estimated to amount up to 6 ppb. This indicates the downward transport of air masses that have been denitrified during the earlier winter phase. Observations within POLSTRACC, at the bottom of the vortex, reflect heterogeneous processes from the overlying Arctic winter stratosphere. The comparison of the observations with CLaMS model simulations confirm and complete the picture arising from the present measurements. The simulations confirm, that the ensemble of all observations is representative for the vortex-wide vertical NOy-redistribution. [ABSTRACT FROM AUTHOR]

The Asian Monsoon Anticyclone (AMA) represents the wettest region in the lower stratosphere (LS) and is the key contributor to the global annual maximum in LS water vapour. While the AMA wet pool is linked with persistent convection in the region and horizontal confinement of the anticyclone, there remain ambiguities regarding the role of tropopause-overshooting convection in maintaining the regional LS water vapour maximum. This study tackles this issue using a unique set of observations from onboard the high-altitude M55-Geophysica aircraft deployed in Nepal in Summer 2017 within the EU StratoClim project. We use a combination of airborne measurements (water vapour, ice water, water isotopes, cloud backscatter) together with ensemble trajectory modeling coupled with satellite observations to characterize the processes controlling water vapour and clouds in the confined lower stratosphere (CLS) of AMA. Our analysis puts in evidence the dual role of overshooting convection, which may lead to hydration or dehydration depending on the synoptic-scale tropopause temperatures in AMA. We show that all of the observed CLS water vapour enhancements are traceable to convective events within AMA and furthermore bear an isotopic signature of the overshooting process. A surprising result is that the plumes of moist air with mixing ratios nearly twice the background level can persist for weeks whilst recirculating within the anticyclone, without being subject to irreversible dehydration through ice settling. Our findings highlight the importance of convection and recirculation within AMA for the transport of water into the stratosphere. [ABSTRACT FROM AUTHOR]

The Asian summer monsoon is an effective pathway for aerosol particles and precursor substances 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) has been observed by satellites, called the Asian Tropopause Aerosol Layer (ATAL). In this paper we discuss airborne in situ and remote sensing observations of aerosol microphysical properties conducted during the 2017 StratoClim field campaign within the region of the Asian monsoon anticyclone. The aerosol particle measurements aboard the high-altitude research aircraft M55 Geophysica (reached a maximum altitude of about 20.5 km) were conducted by a modified Ultra High Sensitivity Aerosol Spectrometer Airborne (UHSAS-A; particle diameter detection range from 65 nm to 1 µm), the COndensation PArticle counting System (COPAS, for detecting total aerosol densities of submicrometer sized particles), and the Cloud and Aerosol Spectrometer with Detection of POLarization (NIXE-CAS -DPOL). In the COPAS and UHSAS-A vertical particle mixing ratio profiles, the ATAL is evident as a distinct layer between 15 km (≈ 370 K) and 18.5 km altitude (≈ 420 K potential temperature). Within the ATAL, the maximum detected particle mixing ratios (from the median profiles) were 700 mg-1 for diameters between 65 nm to 1 µm (UHSAS-A) and higher than 2500 mg-1 for diameters larger than 10 nm (COPAS). These values are up to two times higher than previously found at similar altitudes in other tropical locations. The difference between the particle mixing ratio profiles measured by the UHSAS-A and the COPAS indicate that the region below the ATAL at potential temperatures from 350 to 370 K is influenced by the fresh nucleation of aerosol particles (diameter < 65 nm). We provide detailed analyses of the vertical distribution of the aerosol particle size distributions and the particle mixing ratios and compare these with previous tropical and extratropical measurements. The aerosol scattering ratio was calculated based on the in situ measured aerosol particle size distributions. The resulting dataset was compared with the vertical profiles of the aerosol scattering ratios 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 each other, showing enhanced values of aerosol scattering ratio in the altitude range of the Asian Tropopause Aerosol Layer 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 aerosol scattering ratio larger 1.08 could only be observed within the confinement of the Asian monsoon anticyclone. [ABSTRACT FROM AUTHOR]

From 27 July to 10 August 2017 the airborne StratoClim mission took place in Kathmandu, Nepal where eight mission flights were conducted with the M-55 Geophysica up to altitudes of 20 km. New Particle Formation (NPF) was identified by the abundant presence of ultrafine aerosols, with particle diameters dp smaller than 15 nm, which were in-situ detected by means of condensation nuclei counting techniques. NPF fields in clear-skies as well as in the presence of cloud ice particles (dp > 3 µm) were encountered at upper troposphere/lowermost stratosphere (UT/LS) levels and within the Asian Monsoon Anticyclone (AMA). NPF-generated ultrafine particles in elevated concentrations (Nuf) were frequently found together with cloud ice (in number concentrations Nice of up to 3 cm-3) at heights between ~ 11 km and 16 km. From a total measurement time of ~ 22.5 hours above 10 km altitude, in-cloud NPF was in sum detected over ~ 1.3 hours (~ 50 % of all NPF records throughout StratoClim). Maximum Nuf of up to ~ 11000 cm-3 were detected coincidentally with intermediate ice particle concentrations Nice of 0.05-0.1 cm-3 at comparatively moderate carbon monoxide (CO) contents of ~ 90-100 nmol mol-1. Neither under clear-sky nor during in-cloud NPF do the highest Nuf concentrations correlate with the highest CO mixing ratios, suggesting that an elevated pollutant load is not a prerequisite for NPF. Under clear-air conditions, NPF with elevated Nuf (> 8000 cm-3) occurred slightly less often than within clouds. In the presence of cloud ice, NPF with Nuf between 1500-4000 cm-3 were observed about twice as often as under clear air conditions. When ice water contents exceeded 1000 µmol mol-1 in very cold air (< 195 K) at tropopause levels NPF was not found. This may indicate a reduction of NPF once a strong overshoot is prevalent together with the presence of mainly liquid-origin ice particles. In the presence of in-situ cirrus near the cold point tropopause very recent NPF or events of remarkable strength (mixing ratios nuf > 5000 mg-1) were rarely observed (~ 6 % of in-cloud NPF data). For specifying the constraining mechanisms for NPF possibly imposed by the microphysical properties of the cloud elements, the integral radius (IR) of the ice cloud population was identified as the most practicable indicator. Neither of both, the number of ice particles or the free distance between the ice particles, is clearly related to the NPF-rate detected. The results of a numerical simulation indicates how the IR affects the supersaturation of a condensable vapour, such as sulphuric acid, and that IR determines the effective limitation of NPF rates due to cloud ice. [ABSTRACT FROM AUTHOR]

This study presents airborne in-situ and satellite remote sensing climatologies of cirrus clouds and humidity. The climatologies serve as a guide to the properties of cirrus clouds, with the new in-situ data base providing detailed insights into boreal mid-latitudes and the tropics, while the satellite-borne data set offers a global overview. To this end, an extensive, quality checked data archive, the Cirrus Guide II in-situ data base, is created from airborne in-situ measurements during 150 flights in 24 campaigns. The archive contains meteorological parameters, IWC, Nice, Rice, RHice and H2O for each of the flights (IWC: ice water content, Nice: number concentration of ice crystals, Rice: ice crystal mean mass radius, RHice: relative humidity with respect to ice, H2O: water vapor mixing ratio). Depending on the specific parameter, the data base has extended by about a factor of 5-10 compared to the previous studies of Schiller et al. (2008), JGR, and Krämer et al. (2009), ACP. One result of our investigations is, that across all latitudes, the thicker liquid origin cirrus predominate at lower altitudes, while at higher altitudes the thinner in-situ cirrus prevail. Further, exemplary investigations of the radiative characteristics of in-situ and liquid origin cirrus show that the in-situ origin cirrus only slightly warm the atmosphere, while liquid origin cirrus have a strong cooling effect. An important step in completing the Cirrus Guide II is the provision of the global cirrus Nice climatology, derived by means of the retrieval algorithm DARDAR-Nice from ten years of cirrus remote sensing observations from satellite. The in-situ data base has been used to evaluate and adjust the satellite observations. We found that the global median Nice from satellite observations is almost two times higher than the in-situ median and increases slightly with decreasing temperature. Nice medians of the most frequentl occuring cirrus sorted by geographical regions are highest in the tropics, followed by austral/boreal mid-latitudes, Antarctica and the Arctic. Since the satellite climatologies enclose the entire spatial and temporal Nice occurrence, we could deduce that half of the cirrus are located in the lowest, warmest cirrus layer and contain a significant amount of liquid origin cirrus. A specific highlight of the study is the in-situ observations of tropical tropopause layer (TTL) cirrus and humidity in the Asian monsoon anticyclone and the comparison to the surrounding tropics. In the convectively very active Asian monsoon, peak values of Nice and IWC of 30 ppmv and 1000 ppmv are detected around the cold point tropopause (CPT). Above the CPT, ice particles that are convectively injected can locally add a significant amount of water available for exchange with the stratosphere. We found IWCs of up to 8 ppmv in the Asian monsoon in comparison to only 2 ppmv in the surrounding tropics. Also, the highest RHice inside of the clouds as well as in clear sky (120-150 %) are observed around and above the CPT. We attribute this to the high amount of H2O (3-5 ppmv) in comparison to 1.5-3 ppmv in other tropical regions. The supersaturations above the CPT suggest that the water exchange with the stratosphere is 10-20 % higher than expected in regions of weak convective activity and up to about 50 % in the Asian monsoon. [ABSTRACT FROM AUTHOR]