0000000000059728
AUTHOR
S. Borrmann
The impact of mineral dust on cloud formation during the Saharan dust event in April 2014 over Europe
A regional modeling study on the impact of desert dust on cloud formation is presented for a major Saharan dust outbreak over Europe from 2 to 5 April 2014. The dust event coincided with an extensive and dense cirrus cloud layer, suggesting an influence of dust on atmospheric ice nucleation. Using interactive simulation with the regional dust model COSMO-MUSCAT, we investigate cloud and precipitation representation in the model and test the sensitivity of cloud parameters to dust–cloud and dust–radiation interactions of the simulated dust plume. We evaluate model results with ground-based and spaceborne remote sensing measurements of aerosol and cloud properties, as well as the in situ meas…
A microphysics guide to cirrus clouds - Part 1: Cirrus types
Abstract. The microphysical and radiative properties of cirrus clouds continue to be beyond understanding and thus still represent one of the largest uncertainties in the prediction of the Earth's climate (IPCC, 2013). Our study aims to provide a guide to cirrus microphysics, which is compiled from an extensive set of model simulations, covering the broad range of atmospheric conditions for cirrus formation and evolution. The model results are portrayed in the same parameter space as field measurements, i.e., in the Ice Water Content-Temperature (IWC-T) parameter space. We validate this cirrus analysis approach by evaluating cirrus data sets from 17 aircraft campaigns, conducted in the last…
Thermodynamic correction of particle concentrations measured by underwing probes on fast-flying aircraft
Particle concentration measurements with underwing probes on aircraft are impacted by air compression upstream of the instrument body as a function of flight velocity. In particular, for fast-flying aircraft the necessity arises to account for compression of the air sample volume. Hence, a correction procedure is needed to invert measured particle number concentrations to ambient conditions that is commonly applicable to different instruments to gain comparable results. In the compression region where the detection of particles occurs (i.e. under factual measurement conditions), pressure and temperature of the air sample are increased compared to ambient (undisturbed) conditions in certain …
Aerosol properties, source identification, and cloud processing in orographic clouds measured by single particle mass spectrometry on a central European mountain site during HCCT-2010
Cloud residues and out-of-cloud aerosol particles with diameters between 150 and 900 nm were analysed by online single particle aerosol mass spectrometry during the 6-week study Hill Cap Cloud Thuringia (HCCT)-2010 in September–October 2010. The measurement location was the mountain Schmücke (937 m a.s.l.) in central Germany. More than 160 000 bipolar mass spectra from out-of-cloud aerosol particles and more than 13 000 bipolar mass spectra from cloud residual particles were obtained and were classified using a fuzzy c-means clustering algorithm. Analysis of the uncertainty of the sorting algorithm was conducted on a subset of the data by comparing the clustering output with particle-by-par…
Spectral optical layer properties of cirrus from collocated airborne measurements and simulations
Abstract. Spectral upward and downward solar irradiances from vertically collocated measurements above and below a cirrus layer are used to derive cirrus optical layer properties such as spectral transmissivity, absorptivity, reflectivity, and cloud top albedo. The radiation measurements are complemented by in situ cirrus crystal size distribution measurements and radiative transfer simulations based on the microphysical data. The close collocation of the radiative and microphysical measurements, above, beneath, and inside the cirrus, is accomplished by using a research aircraft (Learjet 35A) in tandem with the towed sensor platform AIRTOSS (AIRcraft TOwed Sensor Shuttle). AIRTOSS can be re…
Sub-micrometer refractory carbonaceous particles in the polar stratosphere
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 i…
Variability of aerosol, gaseous pollutants and meteorological characteristics associated with changes in air mass origin at the SW Atlantic coast of Iberia
Measurements of the ambient aerosol were performed at the Southern coast of Spain, within the framework of the DOMINO (<b>D</b>iel <b>O</b>xidant <b>M</b>echanisms <b>I</b>n relation to <b>N</b>itrogen <b>O</b>xides) project. The field campaign took place from 20 November until 9 December 2008 at the atmospheric research station "El Arenosillo" (37°5'47.76" N, 6°44'6.94" W). As the monitoring station is located at the interface between a natural park, industrial cities (Huelva, Seville) and the Atlantic Ocean, a variety of physical and chemical parameters of aerosols and gas phase could be characterized in dependency on…
Comparison of aircraft measurements during GoAmazon2014/5 and ACRIDICON-CHUVA
Abstract. The indirect effect of atmospheric aerosol particles on the Earth's radiation balance remains one of the most uncertain components affecting climate change throughout the industrial period. The large uncertainty is partly due to the incomplete understanding of aerosol–cloud interactions. One objective of the GoAmazon2014/5 and the ACRIDICON (Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems)-CHUVA (Cloud Processes of the Main Precipitation Systems in Brazil) projects was to understand the influence of emissions from the tropical megacity of Manaus (Brazil) on the surrounding atmospheric environment of the rainforest and to investiga…
In situ observation of new particle formation (NPF) in the tropical tropopause layer of the 2017 Asian monsoon anticyclone - Part 2: NPF inside ice clouds
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 nucleation-mode aerosols, with particle diameters dp smaller than 15 nm, which were in-situ-detected by means of condensation nuclei (CN) counter 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 (UTLS) levels and within the Asian monsoon anticyclone (AMA). NPF-generated nucleation-mode particles in elevated concentration…
Mass-spectrometric identification of primary biological particle markers and application to pristine submicron aerosol measurements in Amazonia
The detection of primary biological material in submicron aerosol by means of thermal desorption/electron impact ionization aerosol mass spectrometry was investigated. Mass spectra of amino acids, carbohydrates, small peptides, and proteins, all of which are key building blocks of biological particles, were recorded in laboratory experiments. Several characteristic marker fragments were identified. The intensity of the marker signals relative to the total organic mass spectrum allows for an estimation of the content of primary biological material in ambient organic aerosol. The developed method was applied to mass spectra recorded during AMAZE-08, a field campaign conducted in the pristine …
Aircraft-based observations of isoprene-epoxydiol-derived secondary organic aerosol (IEPOX-SOA) in the tropical upper troposphere over the Amazon region
During the ACRIDICON-CHUVA field project (September–October 2014; based in Manaus, Brazil) aircraft-based in situ measurements of aerosol chemical composition were conducted in the tropical troposphere over the Amazon using the High Altitude and Long Range Research Aircraft (HALO), covering altitudes from the boundary layer (BL) height up to 14.4 km. The submicron non-refractory aerosol was characterized by flash-vaporization/electron impact-ionization aerosol particle mass spectrometry. The results show that significant secondary organic aerosol (SOA) formation by isoprene oxidation products occurs in the upper troposphere (UT), leading to increased organic aerosol mass concentratio…
Particulate trimethylamine in the summertime Canadian high Arctic lower troposphere
Size-resolved and vertical profile measurements of single particle chemical composition (sampling altitude range 50–3000 m) were conducted in July 2014 in the Canadian high Arctic during an aircraft-based measurement campaign (NETCARE 2014). We deployed the single particle laser ablation aerosol mass spectrometer ALABAMA (vacuum aerodynamic diameter range approximately 200–1000 nm) to identify different particle types and their mixing states. On the basis of the single particle analysis, we found that a significant fraction (23 %) of all analyzed particles (in total: 7412) contained trimethylamine (TMA). Two main pieces of evidence suggest that these TMA-containing particles originated from…
Porous aerosol in degassing plumes of Mt. Etna and Mt. Stromboli
Abstract. Aerosols of the volcanic degassing plumes from Mt. Etna and Mt. Stromboli were probed with in situ instruments on board the Deutsches Zentrum für Luft- und Raumfahrt research aircraft Falcon during the contrail, volcano, and cirrus experiment CONCERT in September 2011. Aerosol properties were analyzed using angular scattering intensities and particle size distributions simultaneously measured with the Polar Nephelometer and the Forward Scattering Spectrometer probes (FSSP series 100 and 300), respectively. Aerosols of degassing plumes are characterized by low values of the asymmetry parameter (between 0.6 and 0.75); the effective diameter was within the range of 1.5–2.8 µm and the…
A tandem approach for collocated measurements of microphysical and radiative cirrus properties
Microphysical and radiation measurements were collected with the novel AIRcraft TOwed Sensor Shuttle (AIRTOSS) – Learjet tandem platform. The platform is a combination of an instrumented Learjet 35A research aircraft and an aerodynamic bird, which is detached from and retracted back to the aircraft during flight via a steel wire with a length of 4000 m. Both platforms are equipped with radiative, cloud microphysical, trace gas, and meteorological instruments. The purpose of the development of this tandem set-up is to study the inhomogeneity of cirrus as well as other stratiform clouds. Sophisticated numerical flow simulations were conducted in order to optimally integrate an axially asymmet…
Illustration of microphysical processes in Amazonian deep convective clouds in the gamma phase space: introduction and potential applications
Abstract. The behavior of tropical clouds remains a major open scientific question, resulting in poor representation by models. One challenge is to realistically reproduce cloud droplet size distributions (DSDs) and their evolution over time and space. Many applications, not limited to models, use the gamma function to represent DSDs. However, even though the statistical characteristics of the gamma parameters have been widely studied, there is almost no study dedicated to understanding the phase space of this function and the associated physics. This phase space can be defined by the three parameters that define the DSD intercept, shape, and curvature. Gamma phase space may provide a commo…
Aerosol quantification with the Aerodyne Aerosol Mass Spectrometer: detection limits and ionizer background effects
Systematic laboratory experiments were performed to investigate quantification of various species with two versions of the Aerodyne Aerosol Mass Spectrometer, a Quadrupole Aerosol Mass Spectrometer (Q-AMS) and a compact Time-of-Flight Aerosol Mass Spectrometer (c-ToF-AMS). Here we present a new method to continuously determine the detection limits of the AMS analyzers during regular measurements, yielding detection limit (<i>DL</i>) information under various measurement conditions. Minimum detection limits range from 0.03 μg m<sup>&minus;3</sup> (nitrate, sulfate, and chloride) up to 0.5 μg m<sup>&minus;3</sup> (organics) for the Q-AMS. Those of t…
Quantitative single-particle analysis with the Aerodyne aerosol mass spectrometer: development of a new classification algorithm and its application to field data
Single-particle mass spectrometry has proven a valuable tool for gaining information on the mixing state of aerosol particles. With the Aerodyne aerosol mass spectrometer (AMS) equipped with a light-scattering probe, non-refractory components of submicron particles with diameters larger than about 300 nm can even be quantified on a single-particle basis. Here, we present a new method for the analysis of AMS single-particle mass spectra. The developed algorithm classifies the particles according to their components (e.g. sulphate, nitrate, different types of organics) and simultaneously provides quantitative information about the composition of the single particles. This classification algor…
The ATAL within the 2017 Asian Monsoon Anticyclone: Microphysical aerosol properties derived from aircraft-borne in situ measurements
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 about 20.5 km) were conducted with a m…
Aerosol particle measurements at three stationary sites in the megacity of Paris during summer 2009: meteorology and air mass origin dominate aerosol particle composition and size distribution
During July 2009, a one-month measurement campaign was performed in the megacity of Paris. Amongst other measurement platforms, three stationary sites distributed over an area of 40 km in diameter in the greater Paris region enabled a detailed characterization of the aerosol particle and gas phase. Simulation results from the FLEXPART dispersion model were used to distinguish between different types of air masses sampled. It was found that the origin of air masses had a large influence on measured mass concentrations of the secondary species particulate sulphate, nitrate, ammonium, and oxygenated organic aerosol measured with the Aerodyne aerosol mass spectrometer in the submicron particle …
Thermodynamic correction of particle concentrations measured by underwing probes on fast flying aircraft
Abstract. Particle concentration measurements with underwing probes on aircraft are impacted by air compression upstream of the instrument body as a function of flight velocity. In particular for fast-flying aircraft the necessity arises to account for compression of the air sample volume. Hence, a correction procedure is needed to invert measured particle number concentrations to ambient conditions that is commonly applicable for different instruments to gain comparable results. In the compression region where the detection of particles occurs (i.e. under factual measurement conditions), pressure and temperature of the air sample are increased compared to ambient (undisturbed) conditions i…
Design of a mobile aerosol research laboratory and data processing tools for effective stationary and mobile field measurements
A compact mobile aerosol research laboratory (MoLa) for stationary and mobile measurements of aerosol and trace gas characteristics was developed at the Max Planck Institute for Chemistry (MPIC) in Mainz, Germany. Major efforts were made to design an aerosol inlet system which is optimized and characterised for both, stationary and mobile measurements using a particle loss modelling approach. The instrumentation on board allows the determination of a multitude of physical and chemical aerosol parameters, for example particle number and mass concentration (PM<sub>1/2.5/10</sub>), particle size distributions in the diameter range 6 nm up to 32 μm, and chemical composition of the s…
Tropical deep convective life cycle : Cb-anvil cloud microphysics from high-altitude aircraft observations
The case study presented here focuses on the life cycle of clouds in the anvil region of a tropical deep convective system. During the SCOUT-O3 campaign from Darwin, Northern Australia, the Hector storm system has been probed by the Geophysica high-altitude aircraft. Clouds were observed by in situ particle probes, a backscatter sonde, and a miniature lidar. Additionally, aerosol number concentrations have been measured. On 30 November 2005 a double flight took place and Hector was probed throughout its life cycle in its developing, mature, and dissipating stage. The two flights were four hours apart and focused on the anvil region of Hector in altitudes between 10.5 and 18.8 km (i.e. above…
Microphysical properties of synoptic scale polar stratospheric clouds: in situ measurements of unexpectedly large HNO&lt;sub&gt;3&lt;/sub&gt; containing particles in the Arctic vortex
Abstract. In January 2010 and December 2011 synoptic scale PSC fields were probed during seven flights of the high altitude research aircraft M-55 Geophysica within the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interaction.) and the ESSenCe (ESSenCe: ESA Sounder Campaign) projects. Particle size distributions in a diameter range between 0.46 μm and 40 μm were recorded simultaneously by up to four different optical in situ instruments. Three of these particle instruments are based on the detection of forward scattered light by single particles. The fourth instrument is a grey scale optical array…
Quantitative single particle analysis with the Aerodyne aerosol mass spectrometer: development of a new classification algorithm and its application to field data
Abstract. Single particle mass spectrometry has proven a valuable tool for gaining information on the mixing state of aerosol particles. With the Aerodyne aerosol mass spectrometer (AMS) equipped with a light scattering probe, non-refractory components of submicron particles with diameters larger than about 300 nm can even be quantified on a single particle basis. Here, we present a new method for the analysis of AMS single particle mass spectra. The developed algorithm classifies the particles according to their components (e.g., sulphate, nitrate, different types of organics) and simultaneously provides quantitative information about the composition of the single particles. This classific…
Aerosol characteristics and particle production in the upper troposphere over the Amazon Basin
Airborne observations over the Amazon Basin showed high aerosol particle concentrations in the upper troposphere (UT) between 8 and 15 km altitude, with number densities (normalized to standard temperature and pressure) often exceeding those in the planetary boundary layer (PBL) by 1 or 2 orders of magnitude. The measurements were made during the German–Brazilian cooperative aircraft campaign ACRIDICON–CHUVA, where ACRIDICON stands for Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems and CHUVA is the acronym for Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM …
Influence of vessel characteristics and atmospheric processes on the gas and particle phase of ship emission plumes: in situ measurements in the Mediterranean Sea and around the Arabian Peninsula
A total of 252 emission plumes of ships operating in the Mediterranean Sea and around the Arabian Peninsula were investigated using a comprehensive dataset of gas- and submicron-particle-phase properties measured during the 2-month shipborne AQABA (Air Quality and Climate Change in the Arabian Basin) field campaign in summer 2017. The post-measurement identification of the corresponding ship emission events in the measured data included the determination of the plume sources (up to 38 km away) as well as the plume ages (up to 115 min) and was based on commercially available historical records of the Automatic Identification System. The dispersion lifetime of chemically inert C…
Influx of African biomass burning aerosol during the Amazonian dry season through layered transatlantic transport of black carbon-rich smoke
Black carbon (BC) aerosols influence the Earth's atmosphere and climate, but their microphysical properties, spatiotemporal distribution, and long-range transport are not well constrained. This study presents airborne observations of the transatlantic transport of BC-rich African biomass burning (BB) smoke into the Amazon Basin using a Single Particle Soot Photometer (SP2) as well as several complementary techniques. We base our results on observations of aerosols and trace gases off the Brazilian coast onboard the HALO (High Altitude and LOng range) research aircraft during the ACRIDICON-CHUVA campaign in September 2014. During flight AC19 over land and ocean at the northeastern coastline …
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
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−…
The ion trap aerosol mass spectrometer: field intercomparison with the ToF-AMS and the capability of differentiating organic compound classes via MS-MS
Further development and optimisation of a previously described ion trap aerosol mass spectrometer (IT-AMS) are presented, which resulted in more reproducible and robust operation and allowed for the instrument's first field deployment. Results from this 11-day-long measurement indicate that the instrument is capable of providing quantitative information on organics, nitrate, and sulfate mass concentrations with reasonable detection limits (0.5–1.4 µg m−3 for 1 h averages) and that results obtained with the IT-AMS can directly be related to those from Aerodyne aerosol mass spectrometers. The capability of the IT-AMS to elucidate the structure of fragment ions is demonstrated via an MS4 study…
Aerosol properties, source identification, and cloud processing in orographic clouds measured by single particle mass spectrometry on a Central European mountain site during HCCT-2010
Abstract. Cloud residues and out-of-cloud aerosol particles with diameters between 150 and 900 nm have been analysed by on-line single particle aerosol mass spectrometry during the six-week study HCCT-2010 in September/October 2010. The measurement location was the mountain Schmücke (937 m a.s.l.) in Central Germany. More than 170 000 bipolar mass spectra from out-of-cloud aerosol particles and more than 14 000 bipolar mass spectra from cloud residual particles were obtained and were classified using a fuzzy c-means clustering algorithm. Analysis of the uncertainty of the sorting algorithm was conducted on a subset of the data by comparing the clustering output with particle-by-particle ins…
Megacity emission plume characteristics in summer and winter investigated by mobile aerosol and trace gas measurements: the Paris metropolitan area
For the investigation of megacity emission plume characteristics mobile aerosol and trace gas measurements were carried out in the greater Paris region in July 2009 and January–February 2010 within the EU FP7 MEGAPOLI project (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation). The deployed instruments measured physical and chemical properties of sub-micron aerosol particles, gas phase constituents of relevance for urban air pollution studies and meteorological parameters. The emission plume was identified based on fresh pollutant (e.g., particle-bound polycyclic aromatic hydrocarbons, black carbon…
Small ice particles at slightly supercooled temperatures in tropical maritime convection
In this paper we show that the origin of the ice phase in tropical cumulus clouds over the sea may occur by primary ice nucleation of small crystals at temperatures just between 0 and −5 ∘C. This was made possible through use of a holographic instrument able to image cloud particles at very high resolution and small size (6 µm). The environment in which the observations were conducted was notable for the presence of desert dust advected over the ocean from the Sahara. However, there is no laboratory evidence to suggest that these dust particles can act as ice nuclei at temperatures warmer than about −10 ∘C, the zone in which the first ice was observed in these clouds. T…