0000000000160780
AUTHOR
Joachim Curtius
Partitioning of Aerosol Particles in Mixed-phase Clouds at a High Alpine Site
6 German Aerospace Centre, D-82234, Wessling, Germany * Now at Institute for Atmospheric and Climate Science, ETH Zurich, 8092 Zurich, Switzerland Abstract The partitioning of aerosol particles between the cloud and the interstitial phase (i.e., unactivated aerosol) has been investigated during several Cloud and Aerosol Characterization Experiments (CLACE) conducted in winter and summer 2004 and winter 2005 at the high alpine research station Jungfraujoch (3,580 m altitude, Switzerland). Ambient air was sampled using different inlets in order to determine the scavenged fraction of aerosol particles, F Scav , and of black carbon, F Scav,BC . They denote the fraction of the aerosol volume con…
In situ observations of new particle formation in the tropical upper troposphere: the role of clouds and the nucleation mechanism
New particle formation (NPF), which generates nucleation mode aerosol, was observed in the tropical Upper Troposphere (UT) and Tropical Tropopause Layer (TTL) by in situ airborne measurements over South America (January–March 2005), Australia (November–December 2005), West Africa (August 2006) and Central America (2004–2007). Particularly intense NPF was found at the bottom of the TTL. Measurements with a set of condensation particle counters (CPCs) with different <i>d</i><sub>p50</sub> (50% lower size detection efficiency diameter or "cut-off diameter") were conducted on board the M-55 <i>Geophysica</i> in the altitude range of 12.0–20.5 km and on board …
The ACRIDICON-CHUVA campaign: Studying tropical deep convective clouds and precipitation over Amazonia using the new German research aircraft HALO
Abstract Between 1 September and 4 October 2014, a combined airborne and ground-based measurement campaign was conducted to study tropical deep convective clouds over the Brazilian Amazon rain forest. The new German research aircraft, High Altitude and Long Range Research Aircraft (HALO), a modified Gulfstream G550, and extensive ground-based instrumentation were deployed in and near Manaus (State of Amazonas). The campaign was part of the German–Brazilian 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 Precipitatio…
Comparison of Two Aerodynamic Lenses as an Inlet for a Single Particle Laser Ablation Mass Spectrometer
By means of a newly designed portable aerosol mass spectrometer SPLAT (Single Particle Laser Ablation Time-of-flight mass spectrometer) for the analysis of single atmospheric aerosol particles we investigated the system performance in dependency on two different aerodynamic lenses (Liu and Schreiner type) capable of focusing particles with diameters ranging from 80 nm to 800 nm and 300 nm to 3000 nm, respectively. By using the pressure regulated Schreiner lens, the instrument is independent of variations in atmospheric pressure which would lead to changing dynamical properties of the aerosol particles. Active pressure control inside the inlet system facilitates airborne measurements without…
A comprehensive characterization of ice nucleation by three different types of cellulose particles immersed in water: lessons learned and future research directions
We present the laboratory results of immersion freezing efficiencies of cellulose particles at supercooled temperature (T) conditions. Three types of chemically homogeneous cellulose samples are used as surrogates that represent supermicron and submicron ice nucleating plant structural polymers. These samples include micro-crystalline cellulose (MCC), fibrous cellulose (FC) and nano-crystalline cellulose (NCC). Our experimental data show that particles resembling the MCC lab particle occur also in the atmosphere. Our immersion freezing dataset includes data from various ice nucleation measurement techniques available at seventeen different institutions, including nine dry dispersion and ele…
Size Matters More Than Chemistry for Cloud-Nucleating Ability of Aerosol Particles
Size-resolved cloud condensation nuclei (CCN) spectra measured for various aerosol types at a non-urban site in Germany showed that CCN concentrations are mainly determined by the aerosol number size distribution. Distinct variations of CCN activation with particle chemical composition were observed but played a secondary role. When the temporal variation of chemical effects on CCN activation is neglected, variation in the size distribution alone explains 84 to 96% of the variation in CCN concentrations. Understanding that particles' ability to act as CCN is largely controlled by aerosol size rather than composition greatly facilitates the treatment of aerosol effects on cloud physics in re…
Inadvertent climate modification due to anthropogenic lead
Atmospheric particles are thought to initiate the majority of terrestrial precipitation. Field-based measurements of ice-crystal residues, together with controlled environment experiments on artificial clouds, suggest that anthropogenic lead-containing particles are among the most efficient ice-forming substances in the atmosphere.
Single-particle characterization of ice-nucleating particles and ice particle residuals sampled by three different techniques
Abstract. In the present work, three different techniques to separate ice-nucleating particles (INPs) as well as ice particle residuals (IPRs) from non-ice-active particles are compared. The Ice Selective Inlet (ISI) and the Ice Counterflow Virtual Impactor (Ice-CVI) sample ice particles from mixed-phase clouds and allow after evaporation in the instrument for the analysis of the residuals. The Fast Ice Nucleus Chamber (FINCH) coupled with the Ice Nuclei Pumped Counterflow Virtual Impactor (IN-PCVI) provides ice-activating conditions to aerosol particles and extracts the activated particles for analysis. The instruments were run during a joint field campaign which took place in January and …
Characterization of a Modified Expansion Condensation Particle Counter for Detection of Nanometer-Sized Particles
A newly developed condensation particle counter provides measurements of aerosol particle number densities for size diameters as low as 3 nm. This Expansion Condensation Particle Counter (ECPC) operates based on fast adiabatic expansion with specialized detection and evaluation of the temporal development of light scattered by the ensemble of growing droplets. In its new configuration the ECPC has been modified such that a previously needed calibration factor became obsolete. In this article the new design is described which now includes a fast pressure sensor for monitoring the pressure drop inside the measurement chamber. Extensive laboratory experiments for characterizing the ECPC are de…
Detection of security relevant substances within the cooperative project SAFE XUV
The objective of this project funded by the German BMBF was to show that security relevant substances can be detected in complex matrices at low concentrations using single photon ionization ion trap mass spectrometry (SPI-ITMS). The advantage of such a soft ionization technique is a reduction of unwanted fragment ions in mass spectra allowing identification of signals from complex matrices and enabling MS/MS capability. The MS/MS studies permit low false-positive and false-negative rates. Additionally, the accumulation of the ions in the ion trap decreases the detection limit. To obtain low detection limits the ionization potentials (IPs) of the relevant substances have to be below the IPs…
ML-CIRRUS: The Airborne Experiment on Natural Cirrus and Contrail Cirrus with the High-Altitude Long-Range Research Aircraft HALO
Abstract The Midlatitude Cirrus experiment (ML-CIRRUS) deployed the High Altitude and Long Range Research Aircraft (HALO) to obtain new insights into nucleation, life cycle, and climate impact of natural cirrus and aircraft-induced contrail cirrus. Direct observations of cirrus properties and their variability are still incomplete, currently limiting our understanding of the clouds’ impact on climate. Also, dynamical effects on clouds and feedbacks are not adequately represented in today’s weather prediction models. Here, we present the rationale, objectives, and selected scientific highlights of ML-CIRRUS using the G-550 aircraft of the German atmospheric science community. The first combi…
Single particle characterization of black carbon aerosols at a tropospheric alpine site in Switzerland
The refractory black carbon (rBC) mass, size distribution (190–720 nm) and mixing state in sub-micron aerosols were characterized from late February to March 2007 using a single particle incandescence method at the high alpine research station Jungfraujoch (JFJ), Switzerland (46.33° N, 7.59° E, 3580 m a.s.l.). JFJ is a ground based location, which is at times exposed to continental free tropospheric air. A median mass absorption coefficient (MAC) of 10.2&plusmn;3.2 m<sup>2</sup> g<sup>−1</sup> at &lambda;=630 nm was derived by comparing single particle incandescence measurements of black carbon mass with continuous measurements of absorption coefficient. This…
Chemical composition of ambient aerosol, ice residues and cloud droplet residues in mixed-phase clouds: single particle analysis during the Cloud and Aerosol Characterization Experiment (CLACE 6)
Abstract. Two different single particle mass spectrometers were operated in parallel at the Swiss High Alpine Research Station Jungfraujoch (JFJ, 3580 m a.s.l.) during the Cloud and Aerosol Characterization Experiment (CLACE 6) in February and March 2007. During mixed phase cloud events ice crystals from 5–20 μm were separated from larger ice aggregates, non-activated, interstitial aerosol particles and supercooled droplets using an Ice-Counterflow Virtual Impactor (Ice-CVI). During one cloud period supercooled droplets were additionally sampled and analyzed by changing the Ice-CVI setup. The small ice particles and droplets were evaporated by injection into dry air inside the Ice-CVI. The …
A comprehensive laboratory study on the immersion freezing behavior of illite NX particles: a comparison of 17 ice nucleation measurement techniques
Immersion freezing is the most relevant heterogeneous ice nucleation mechanism through which ice crystals are formed in mixed-phase clouds. In recent years, an increasing number of laboratory experiments utilizing a variety of instruments have examined immersion freezing activity of atmospherically relevant ice-nucleating particles. However, an intercomparison of these laboratory results is a difficult task because investigators have used different ice nucleation (IN) measurement methods to produce these results. A remaining challenge is to explore the sensitivity and accuracy of these techniques and to understand how the IN results are potentially influenced or biased by experimental param…
Observations of meteoric material and implications for aerosol nucleation in the winter Arctic lower stratosphere derived from in situ particle measurements
Number concentrations of total and non-volatile aerosol particles with size diameters >0.01 μm as well as particle size distributions (0.4–23 μm diameter) were measured in situ in the Arctic lower stratosphere (10–20.5 km altitude). The measurements were obtained during the campaigns European Polar Stratospheric Cloud and Lee Wave Experiment (EUPLEX) and Envisat-Arctic-Validation (EAV). The campaigns were based in Kiruna, Sweden, and took place from January to March 2003. Measurements were conducted onboard the Russian high-altitude research aircraft Geophysica using the low-pressure Condensation Nucleus Counter COPAS (COndensation PArticle Counter System) and a modified F…
Characterization of a Newly Developed Aircraft-Based Laser Ablation Aerosol Mass Spectrometer (ALABAMA) and First Field Deployment in Urban Pollution Plumes over Paris During MEGAPOLI 2009
We present here the development and first field deployment of a novel Aircraft-based Laser ABlation Aerosol MAss spectrometer (ALABAMA), which is capable of measuring the chemical composition and size of individual ambient aerosol particles in the size range between 150 and 900 nm. The instrument uses a continuous wave 532 nm laser to size and detect the particles, a pulsed 266 nm laser to ablate and ionize the particles, and a bipolar, Z-shaped time-of-flight mass spectrometer to detect positive and negative ions. The ALABAMA fits into a 19"-aircraft rack of 150 cm height and has a total weight of 140 kg, thus currently being one of the smallest and lightest-weight instruments of its type.…
Intercomparing different devices for the investigation of ice nucleating particles using Snomax&lt;sup&gt;®&lt;/sup&gt; as test substance
Abstract. Seven different instruments and measurement methods were used to examine the immersion freezing of bacterial ice nuclei from Snomax® (hereafter Snomax), a product containing ice-active protein complexes from non-viable Pseudomonas syringae bacteria. The experimental conditions were kept as similar as possible for the different measurements. Of the participating instruments, some examined droplets which had been made from suspensions directly, and the others examined droplets activated on previously generated Snomax particles, with particle diameters of mostly a few hundred nanometers and up to a few micrometers in some cases. Data were obtained in the temperature range from −2 to …
Enhanced organic mass fraction and decreased hygroscopicity of cloud condensation nuclei (CCN) during new particle formation events
In a forested near-urban location in central Germany, the CCN efficiency of particles smaller than 100 nm decreases significantly during periods of new particle formation. This results in an increase of average activation diameters, ranging from 5 to 8% at supersaturations of 0.33% and 0.74%, respectively. At the same time, the organic mass fraction in the sub-100-nm size range increases from approximately 2/3 to 3/4. This provides evidence that secondary organic aerosol (SOA) components are involved in the growth of new particles to larger sizes, and that the reduced CCN efficiency of small particles is caused by the low hygroscopicity of the condensing material. The observed dependence of…
Nitric Acid Trihydrate (NAT) formation at low NAT supersaturation in Polar Stratospheric Clouds (PSCs)
International audience; A PSC was detected on 6 February 2003 in the Arctic stratosphere by in-situ measurements onboard the high-altitude research aircraft Geophysica. Low number densities (~10-4cm-3) of small nitric acid (HNO3) containing particles (dTNAT, these NAT particles have the potential to grow further and to remove HNO3 from the stratosphere, thereby enhancing polar ozone loss. Interestingly, the NAT particles formed in less than a day at temperatures just slightly below TNAT (T>TNAT-3.1K). This unique measurement of PSC formation at extremely low NAT saturation ratios (SNAT?10) constrains current NAT nucleation theories. We suggest, that the NAT particles have formed heterogeneo…
Quantifying transport into the lowermost stratosphere using simultaneous in-situ measurements of SF&lt;sub&gt;6&lt;/sub&gt; and CO&lt;sub&gt;2&lt;/sub&gt;
Abstract. The seasonality of transport and mixing of air into the lowermost stratosphere (LMS) is studied using distributions of mean age of air and a mass balance approach, based on in-situ observations of SF6 and CO2 during the SPURT (Spurenstofftransport in der Tropopausenregion, trace gas transport in the tropopause region) aircraft campaigns. Combining the information of the mean age of air and the water vapour distributions we demonstrate that the tropospheric air transported into the LMS above the extratropical tropopause layer (ExTL) originates predominantly from the tropical tropopause layer (TTL). The concept of our mass balance is based on simultaneous measurements of the two pas…
HNO3 partitioning in cirrus clouds
During the 1997 POLSTAR-1 winter campaign in northern Sweden a flight was performed across a cold trough of air (similar or equal to 196 K) in the tropopause region. Measurements of total water vapour, nitric acid, particles and reactive nitrogen (NOy) were taken. The particle measurements indicate that about 3% of the particles in the moist tropospheric air were ice particles. Forward and backward facing NOy inlets were used simultaneously to determine condensed phase HNO3. The combined NOy and particle measurements reveal that less than 1% of a monolayer of NOy could have resided on the ice particles. This casts doubt on the hypothesis that sedimenting cirrus particles generally lead to a…