ALBERT

Description: Eleven particle samples collected in the polar stratosphere during SOLVE (SAGE III Ozone loss and validation experiment) from January until March 2000 were characterized in detail by high-resolution transmission and scanning electron microscopy (TEM/SEM) combined with energy-dispersive X-ray microanalysis. A total of 4202 particles (TEM  =  3872; SEM  =  330) were analyzed from these samples, which were collected mostly inside the polar vortex in the altitude range between 17.3 and 19.9 km. Particles that were volatile in the microscope beams contained ammonium sulfates and hydrogen sulfates and dominated the samples. Some particles with diameters ranging from 20 to 830 nm were refractory in the electron beams. Carbonaceous particles containing additional elements to C and O comprised from 72 to 100 % of the refractory particles. The rest were internal mixtures of these materials with sulfates. The median number mixing ratio of the refractory particles, expressed in units of particles per milligram of air, was 1.1 (mg air)−1 and varied between 0.65 and 2.3 (mg air)−1. Most of the refractory carbonaceous particles are completely amorphous, a few of the particles are partly ordered with a graphene sheet separation distance of 0.37 ± 0.06 nm (mean value ± standard deviation). Carbon and oxygen are the only detected major elements with an atomic O∕C ratio of 0.11 ± 0.07. Minor elements observed include Si, S, Fe, Cr and Ni with the following atomic ratios relative to C: Si∕C: 0.010 ± 0.011; S∕C: 0.0007 ± 0.0015; Fe∕C: 0.0052 ± 0.0074; Cr∕C: 0.0012 ± 0.0017; Ni∕C: 0.0006 ± 0.0011 (all mean values ± standard deviation).High-resolution element distribution images reveal that the minor elements are distributed within the carbonaceous matrix; i.e., heterogeneous inclusions are not observed. No difference in size, nanostructure and elemental composition was found between particles collected inside and outside the polar vortex. Based on chemistry and nanostructure, aircraft exhaust, volcanic emissions and biomass burning can certainly be excluded as sources. The same is true for the less probable but globally important sources: wood burning, coal burning, diesel engines and ship emissions. Recondensed organic matter and extraterrestrial particles, potentially originating from ablation and fragmentation, remain as possible sources of the refractory carbonaceous particles studied. However, additional work is required in order to identify the sources unequivocally.

Description: Solar radiation reflected by cirrus and deep convective clouds (DCCs) was measured by the Spectral Modular Airborne Radiation Measurement System (SMART) installed on the German High Altitude and Long Range Research Aircraft (HALO) during the Mid-Latitude Cirrus (ML-CIRRUS) and the Aerosol, Cloud, Precipitation, and Radiation Interaction and Dynamic of Convective Clouds System – Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modelling and to the Global Precipitation Measurement (ACRIDICON-CHUVA) campaigns. On particular flights, HALO performed measurements closely collocated with overpasses of the Moderate Resolution Imaging Spectroradiometer (MODIS) aboard the Aqua satellite. A cirrus cloud located above liquid water clouds and a DCC topped by an anvil cirrus are analyzed in this paper. Based on the nadir spectral upward radiance measured above the two clouds, the optical thickness τ and particle effective radius reff of the cirrus and DCC are retrieved using a radiance ratio technique, which considers the cloud thermodynamic phase, the vertical profile of cloud microphysical properties, the presence of multilayer clouds, and the heterogeneity of the surface albedo. For the cirrus case, the comparison of τ and reff retrieved on the basis of SMART and MODIS measurements yields a normalized mean absolute deviation of up to 1.2 % for τ and 2.1 % for reff. For the DCC case, deviations of up to 3.6 % for τ and 6.2 % for reff are obtained. The larger deviations in the DCC case are mainly attributed to the fast cloud evolution and three-dimensional (3-D) radiative effects. Measurements of spectral upward radiance at near-infrared wavelengths are employed to investigate the vertical profile of reff in the cirrus. The retrieved values of reff are compared with corresponding in situ measurements using a vertical weighting method. Compared to the MODIS observations, measurements of SMART provide more information on the vertical distribution of particle sizes, which allow reconstructing the profile of reff close to the cloud top. The comparison between retrieved and in situ reff yields a normalized mean absolute deviation, which ranges between 1.5 and 10.3 %, and a robust correlation coefficient of 0.82.

Description: We have investigated how aerosols affect the height above cloud base of rain and ice hydrometeor initiation and the subsequent vertical evolution of cloud droplet size and number concentrations in growing convective cumulus. For this purpose we used in situ data of hydrometeor size distributions measured with instruments mounted on HALO aircraft during the ACRIDICON–CHUVA campaign over the Amazon during September 2014. The results show that the height of rain initiation by collision and coalescence processes (Dr, in units of meters above cloud base) is linearly correlated with the number concentration of droplets (Nd in cm−3) nucleated at cloud base (Dr ≈ 5 ⋅ Nd). Additional cloud processes associated with Dr, such as GCCN, cloud, and mixing with ambient air and other processes, produce deviations of  ∼  21 % in the linear relationship, but it does not mask the clear relationship between Dr and Nd, which was also found at different regions around the globe (e.g., Israel and India). When Nd exceeded values of about 1000 cm−3, Dr became greater than 5000 m, and the first observed precipitation particles were ice hydrometeors. Therefore, no liquid water raindrops were observed within growing convective cumulus during polluted conditions. Furthermore, the formation of ice particles also took place at higher altitudes in the clouds in polluted conditions because the resulting smaller cloud droplets froze at colder temperatures compared to the larger drops in the unpolluted cases. The measured vertical profiles of droplet effective radius (re) were close to those estimated by assuming adiabatic conditions (rea), supporting the hypothesis that the entrainment and mixing of air into convective clouds is nearly inhomogeneous. Additional CCN activation on aerosol particles from biomass burning and air pollution reduced re below rea, which further inhibited the formation of raindrops and ice particles and resulted in even higher altitudes for rain and ice initiation.

Description: This study has two objectives: (1) it characterizes contrails at very low temperatures and (2) it discusses convective cirrus in which the contrails occurred. (1) Long-lived contrails and cirrus from overshooting convection are investigated above the tropical tropopause at low temperatures down to −88 °C from measurements with the Russian high-altitude research aircraft M-55 Geophysica, as well as related observations during the SCOUT-O3 field experiment near Darwin, Australia, in 2005. A contrail was observed to persist below ice saturation at low temperatures and low turbulence in the stratosphere for nearly 1 h. The contrail occurred downwind of the decaying convective system Hector of 16 November 2005. The upper part of the contrail formed at 19 km altitude in the tropical lower stratosphere at ∼ 60 % relative humidity over ice at −82 °C. The ∼ 1 h lifetime is explained by engine water emissions, slightly enhanced humidity from Hector, low temperature, low turbulence, and possibly nitric acid hydrate formation. The long persistence suggests large contrail coverage in case of a potential future increase of air traffic in the lower stratosphere. (2) Cirrus observed above the strongly convective Hector cloud on 30 November 2005 was previously interpreted as cirrus from overshooting convection. Here we show that parts of the cirrus were caused by contrails or are mixtures of convective and contrail cirrus. The in situ data together with data from an upward-looking lidar on the German research aircraft Falcon, the CPOL radar near Darwin, and NOAA-AVHRR satellites provide a sufficiently complete picture to distinguish between contrail and convective cirrus parts. Plume positions are estimated based on measured or analyzed wind and parameterized wake vortex descent. Most of the non-volatile aerosol measured over Hector is traceable to aircraft emissions. Exhaust emission indices are derived from a self-match experiment of the Geophysica in the polar stratosphere in 2010. The number of ice particles in the contrails is less than 1 % of the number of non-volatile aerosol particles, possibly because of sublimation losses and undetected very small ice particles. The radar data show that the ice water content in convective overshoots is far higher than measured along the flight path. These findings add insight into overshooting convection and are of relevance with respect to hydration of the lower stratosphere.

Description: The objective of this study is to validate parameterizations that were recently developed for satellite retrievals of cloud condensation nuclei supersaturation spectra, NCCN(S), at cloud base alongside more traditional parameterizations connecting NCCN(S) with cloud base updrafts and drop concentrations. This was based on the HALO aircraft measurements during the ACRIDICON–CHUVA campaign over the Amazon region, which took place in September 2014. The properties of convective clouds were measured with a cloud combination probe (CCP), a cloud and aerosol spectrometer (CAS-DPOL), and a CCN counter onboard the HALO aircraft. An intercomparison of the cloud drop size distributions (DSDs) and the cloud water content (CWC) derived from the different instruments generally shows good agreement within the instrumental uncertainties. To this end, the directly measured cloud drop concentrations (Nd) near cloud base were compared with inferred values based on the measured cloud base updraft velocity (Wb) and NCCN(S) spectra. The measurements of Nd at cloud base were also compared with drop concentrations (Na) derived on the basis of an adiabatic assumption and obtained from the vertical evolution of cloud drop effective radius (re) above cloud base. The measurements of NCCN(S) and Wb reproduced the observed Nd within the measurements uncertainties when the old (1959) Twomey's parameterization was used. The agreement between the measured and calculated Nd was only within a factor of 2 with attempts to use cloud base S, as obtained from the measured Wb, Nd, and NCCN(S). This underscores the yet unresolved challenge of aircraft measurements of S in clouds. Importantly, the vertical evolution of re with height reproduced the observation-based nearly adiabatic cloud base drop concentrations, Na. The combination of these results provides aircraft observational support for the various components of the satellite-retrieved methodology that was recently developed to retrieve NCCN(S) under the base of convective clouds. This parameterization can now be applied with the proper qualifications to cloud simulations and satellite retrievals.

Description: The realistic representation of aerosol–cloud interactions is of primary importance for accurate climate model projections. The investigation of these interactions in strongly contrasting clean and polluted atmospheric conditions in the Amazon region has been one of the motivations for several field campaigns, including the airborne “Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems–Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (Global Precipitation Measurement) (ACRIDICON-CHUVA)” campaign based in Manaus, Brazil, in September 2014. In this work we combine in situ and remotely sensed aerosol, cloud, and atmospheric radiation data collected during ACRIDICON-CHUVA with regional, online-coupled chemistry-transport simulations to evaluate the model's ability to represent the indirect effects of biomass burning aerosol on cloud microphysical and optical properties (droplet number concentration and effective radius). We found agreement between the modeled and observed median cloud droplet number concentration (CDNC) for low values of CDNC, i.e., low levels of pollution. In general, a linear relationship between modeled and observed CDNC with a slope of 0.3 was found, which implies a systematic underestimation of modeled CDNC when compared to measurements. Variability in cloud condensation nuclei (CCN) number concentrations was also underestimated, and cloud droplet effective radii (reff) were overestimated by the model. Modeled effective radius profiles began to saturate around 500 CCN cm−3 at cloud base, indicating an upper limit for the model sensitivity well below CCN concentrations reached during the burning season in the Amazon Basin. Additional CCN emitted from local fires did not cause a notable change in modeled cloud droplet effective radii. Finally, we also evaluate a parameterization of CDNC at cloud base using more readily available cloud microphysical properties, showing that we are able to derive CDNC at cloud base from cloud-side remote-sensing observations.

Description: Eleven particle samples collected in the polar stratosphere during SOLVE (SAGE III Ozone loss and validation experiment) from January until March 2000 were characterized in detail by high-resolution transmission and scanning electron microscopy (TEM/SEM) combined with energy-dispersive X-ray microanalysis. A total number of 4175 particles (TEM = 3845; SEM = 330) was analyzed from these samples which were collected mostly inside the polar vortex in the altitude range between 17.3 and 19.9 km. By particle volume, all samples are dominated by volatile particles (ammonium sulfates/hydrogen sulfates). By number, approximately 28–82 % of the particles are refractory carbonaceous with sizes between 20–830 nm. Internal mixtures of refractory carbonaceous and volatile particles comprise up to 16 %, individual volatile particles about 9 to 72 %. Most of the refractory carbonaceous particles are completely amorphous, a few of the particles are partly ordered with a graphene sheet separation distance of 0.37 ± 0.06 nm (mean value ± standard deviation). Carbon and oxygen are the only detected major elements with an atomic O / C ratio of 0.11 ± 0.07. Minor elements observed include Si, S, Fe, Cr and Ni with the following atomic ratios relative to C: Si / C: 0.010 ± 0.011; S / C: 0.0007 ± 0.0015; Fe / C: 0.0052 ± 0.0074; Cr / C: 0.0012 ± 0.0017; Ni / C: 0.0006 ± 0.0011 (all mean values ± standard deviation). High resolution element distribution images reveal that the minor elements are distributed within the carbonaceous matrix, i.e., heterogeneous inclusions are not observed. No difference in size, nanostructure and elemental composition was found between particles collected inside and outside the polar vortex. Based on chemistry and nanostructure, aircraft exhaust, volcanic emissions and biomass burning can certainly be excluded as source. The same is true for the less probable, but globally important sources: wood burning, coal burning, diesel engines and ship emissions. Rocket exhaust and carbonaceous material from interplanetary dust particles remain as possible sources of the refractory carbonaceous particles studied. However, additional work is required in order to identify the sources unequivocally.

Description: Stratospheric aerosol particles with diameters larger than about 10 nm were collected within the arctic vortex during two polar flight campaigns: RECONCILE in winter 2010 and ESSenCe in winter 2011. Impactors were installed on board of the aircraft M-55 Geophysica, which was operated from Kiruna, Sweden. Flights were performed in a height of up to 21 km and some of the particle samples were taken within distinct polar stratospheric clouds (PSC). The chemical composition, size and morphology of refractory particles were analyzed by scanning electron microscopy and energy-dispersive X-ray microanalysis. During ESSenCe no refractory particles with diameters above 500 nm were sampled. In total 116 small silicate-, Fe-rich-, Pb-rich and aluminum oxide spheres were found. In contrast to ESSenCe early winter, during the late winter RECONCILE mission the air masses were subsiding inside the Arctic winter vortex from upper stratosphere and mesosphere, thus initializing a transport of refractory aerosol particles into the lower stratosphere. During RECONCILE 759 refractory particles with diameters above 500 nm were found consisting of silicates, silicate/carbon mixtures, Fe-rich particles, Ca-rich particles and complex metal mixtures. In the size range below 500 nm additionally the presence of soot was proven. While the data base is still sparse, the general tendency of a lower abundance of refractory particles during PSC events compared to non-PSC situations was observed. The detection of such large refractory particles in the stratosphere, and the fact that these particles were not observed in the particle samples (upper size limit about 5 µm) taken during PSC events, strengthen the hypothesis that such particles are present in the polar stratosphere in late winter and that they can provide a surface for heterogeneous condensation during PSC formation.

Description: We have investigated how pollution aerosols affect the height above cloud base of rain and ice hydrometeor initiation and the subsequent vertical evolution of cloud droplet size and number concentrations in growing convective cumulus. For this purpose we used in-situ data of hydrometeor size distributions measured with instruments mounted on HALO (High Altitude and Long Range Research Aircraft) during the ACRIDICON-CHUVA campaign over the Amazon during September 2014. The results show that the height of rain initiation by collision and coalescence processes (Dr, in units of meters above cloud base) is linearly correlated with the number concentration of droplets (Nd in cm−3) nucleated at cloud base (Dr ≈ 5 Nd). When Nd exceeded values of about 1000 cm−3, Dr became greater than 5000 m, and particles of precipitation size were initiated as ice hydrometeors. Therefore, no liquid water raindrops were observed within growing convective cumulus during polluted conditions. Furthermore, also the formation of ice particles took place at higher altitudes in the clouds in polluted conditions, because the resulting smaller cloud droplets froze at colder temperatures compared to the larger drops in the unpolluted cases. The measured vertical profiles of droplet effective radius (re) were close to those estimated by assuming adiabatic conditions (rea), supporting the hypothesis that the entrainment and mixing of air into convective clouds is almost completely inhomogeneous. Secondary nucleation of droplets on aerosol particles from biomass burning and air pollution reduced re below rea, which further inhibited the formation of raindrops and ice particles and resulted in even higher altitudes for rain and ice initiation.

Description: The realistic representation of cloud-aerosol interactions is of primary importance for accurate climate model projections. The investigation of these interactions in strongly contrasting clean and polluted atmospheric conditions in the Amazon area has been one of the motivations for several field observations, including the airborne Aerosol, Cloud, Precipitation, and Radiation Interactions and DynamIcs of CONvective cloud systems – Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (Global Precipitation Measurement) (ACRIDICON-CHUVA) campaign based in Manaus, Brazil in September 2014. In this work we combine in situ and remotely sensed aerosol, cloud, and atmospheric radiation data collected during ACRIDICON-CHUVA with regional, online-coupled chemistry-transport simulations to evaluate the model’s ability to represent the indirect effects of biomass burning aerosol on cloud microphysical properties (droplet number concentration and effective radius). We found agreement between modeled and observed median cloud droplet number concentrations (CDNC) for low values of CDNC, i.e., low levels of pollution. In general, a linear relationship between modeled and observed CDNC with a slope of two was found, which means a systematic underestimation of modeled CDNC as compared to measurements. Variability in cloud condensation nuclei (CCN) number concentrations and cloud droplet effective radii (reff) was also underestimated by the model. Modeled effective radius profiles began to saturate around 500 CCN per cm3 at cloud base, indicating an upper limit for the model sensitivity well below CCN concentrations reached during the burning season in the Amazon Basin. Regional background aerosol concentrations were sufficiently high such that the additional CCN emitted from local fires did not cause a notable change in modelled cloud microphysical properties. In addition, we evaluate a parameterization of CDNC at cloud base using more readily available cloud microphysical properties, aimed at in situ observations and satellite retrievals. Our study casts doubt on the validity of regional scale modeling studies of the cloud albedo effect in convective situations for polluted situations where the number concentration of CCN is greater than 500 cm−3.