In situ Charakterisierung von kleinen Wolkenpartikeln in Mischphasenwolken

Mischphasenwolken (MPWn) bestehen aus unterkühlten Flüssigwassertröpfchen und aus Eispartikeln, sind thermodynamisch instabil und eine Quelle von Unsicherheiten für Klima- und Wettervorhersagen. Ziel dieser Arbeit ist es, durch die Detektion und Analyse von Wolkenpartikeln in MPWn ein verbessertes Verständnis der Mikrophysik dieser Wolken zu erlangen. Dazu wurden in situ Messungen mit neuartigen optischen Instrumenten durchgeführt, die hochaufgelöste Streumuster von einzelnen Wolkenpartikeln mit Größen im Bereich von wenigen bis zu hundert Mikrometern erzeugen. Die Analyse dieser Streumuster ermöglicht eine detaillierte Charakterisierung von Phase und Morphologie der kleinsten Hydrometeore einer MPW. Diese Untersuchungen liefern wertvolle Hinweise auf bisher nur lückenhaft verstandene mikrophysikalische Prozesse in MPWn. Die Messdaten der vorliegenden Arbeit wurden an der AIDA-Wolkenkammer, auf hochalpinen Bergstationen und an Bord von Flugzeugen über der kanadischen Arktis erhoben. Untersuchungen unter wohldefinierten Laborbedingungen an der Wolkenkammer werden zur Charakterisierung und Kalibrierung der Messegeräte und Analysemethoden verwendet. Im Rahmen der Bergstationsmessungen wurden sehr hohe Anzahlkonzentrationen von kleinen Eispartikeln in MPWn gemessen, die mit der Windgeschwindigkeit korrelieren und vermutlich aus sekundären Eisformationsprozessen an der Erdoberfläche stammen. Bei der flugzeugbasierten Untersuchung von arktischen MPWn wurde die Nachweisgrenze für Eispartikel erreicht. Bei diesen Messungen wurden interessante Merkmale der Tröpfchenpopulation festgestellt. Die gewonnenen Erkenntnisse werden mit den Ergebnissen von Modellrechnungen und anderen Messgeräten verglichen. %Die Messungen im neuartigen Eis-selektiven Einlass zeigen, dass bei ihrem jeweiligen Durchgang, Tröpfchen wie gewünscht entfernt, Eispartikel allerdings auch verändert werden

Cloud chamber experiments on the origin of ice crystal complexity in cirrus clouds

This is an open access article, made available under the terms of the Creative Commons attribution license CC BY 3.0 https://creativecommons.org/licenses/by/3.0/This study reports on the origin of ice crystal complexity and its influence on the angular light scattering properties of cirrus clouds. Cloud simulation experiments were conducted at the AIDA (Aerosol Interactions and Dynamics in the Atmosphere) cloud chamber of the Karlsruhe Institute of Technology (KIT). A new experimental procedure was applied to grow and sublimate ice particles at defined super- and subsaturated ice conditions and for temperatures in the −40 to −60 °C range. The experiments were performed for ice clouds generated via homogeneous and heterogeneous initial nucleation. Ice crystal complexity was deduced from measurements of spatially resolved single particle light scattering patterns by the latest version of the Small Ice Detector (SID-3). It was found that a high ice crystal complexity is dominating the microphysics of the simulated clouds and the degree of this complexity is dependent on the available water vapour during the crystal growth. Indications were found that the crystal complexity is influenced by unfrozen H2SO4/H2O residuals in the case of homogeneous initial ice nucleation. Angular light scattering functions of the simulated ice clouds were measured by the two currently available airborne polar nephelometers; the Polar Nephelometer (PN) probe of LaMP and the Particle Habit Imaging and Polar Scattering (PHIPS-HALO) probe of KIT. The measured scattering functions are featureless and flat in the side- and backward scattering directions resulting in low asymmetry parameters g around 0.78. It was found that these functions have a rather low sensitivity to the crystal complexity for ice clouds that were grown under typical atmospheric conditions. These results have implications for the microphysical properties of cirrus clouds and for the radiative transfer through these clouds.Peer reviewedFinal Published versio

Development and characterization of an ice-selecting pumped counterflow virtual impactor (IS-PCVI) to study ice crystal residuals

Separation of particles that play a role in cloud activation and ice nucleation from interstitial aerosols has become necessary to further understand aerosol-cloud interactions. The pumped counterflow virtual impactor (PCVI), which uses a vacuum pump to accelerate the particles and increase their momentum, provides an accessible option for dynamic and inertial separation of cloud elements. However, the use of a traditional PCVI to extract large cloud hydrometeors is difficult mainly due to its small cut-size diameters ( 100 %), where a mixture of droplets and ice crystals was formed during the expansion experiment. In parallel, the flow conditions of the IS-PCVI were actively controlled, such that it separated ice crystals from a mixture of ice crystals and cloud droplets, which were of diameter  ≥  10 µm. These large ice crystals were passed through the heated evaporation section to remove the water content. Afterwards, the residuals were characterized with a suite of online and offline instruments downstream of the IS-PCVI. These results were used to assess the optimized operating parameters of the device in terms of (1) the critical cut-size diameter, (2) the transmission efficiency and (3) the counterflow-to-input flow ratio. Particle losses were characterized by comparing the residual number concentration to the rejected interstitial particle number concentration. Overall results suggest that the IS-PCVI enables inertial separation of particles with a volume-equivalent particle size in the range of  ~ 10–30 µm in diameter with small inadvertent intrusion (~  5 %) of unwanted particles

Quasi-spherical ice in convective clouds

Homogeneous freezing of supercooled droplets occurs in convective systems in low and midlatitudes. This droplet-freezing process leads to the formation of a large amount of small ice particles, so-called frozen droplets, that are transported to the upper parts of anvil outflows, where they can influence the cloud radiative properties. However, the detailed microphysics and, thus, the scattering properties of these small ice particles are highly uncertain. Here, the link between the microphysical and optical properties of frozen droplets is investigated in cloud chamber experiments, where the frozen droplets were formed, grown, and sublimated under controlled conditions. It was found that frozen droplets developed a high degree of small-scale complexity after their initial formation and subsequent growth. During sublimation, the small-scale complexity disappeared, releasing a smooth and near-spherical ice particle. Angular light scattering and depolarization measurements confirmed that these sublimating frozen droplets scattered light similar to spherical particles: that is, they had angular light-scattering properties similar to water droplets. The knowledge gained from this laboratory study was applied to two case studies of aircraft measurements in midlatitude and tropical convective systems. The in situ aircraft measurements confirmed that the microphysics of frozen droplets is dependent on the humidity conditions they are exposed to (growth or sublimation). The existence of optically spherical frozen droplets can be important for the radiative properties of detraining convective outflows.Peer reviewe

Observation of viscosity transition in α-pinene secondary organic aerosol

Under certain conditions, secondary organic aerosol (SOA) particles can exist in the atmosphere in an amorphous solid or semi-solid state. To determine their relevance to processes such as ice nucleation or chemistry occurring within particles requires knowledge of the temperature and relative humidity (RH) range for SOA to exist in these states. In the Cosmics Leaving Outdoor Droplets (CLOUD) experiment at The European Organisation for Nuclear Research (CERN), we deployed a new in situ optical method to detect the viscous state of α-pinene SOA particles and measured their transition from the amorphous highly viscous state to states of lower viscosity. The method is based on the depolarising properties of laboratory-produced non-spherical SOA particles and their transformation to non-depolarising spherical particles at relative humidities near the deliquescence point. We found that particles formed and grown in the chamber developed an asymmetric shape through coagulation. A transition to a spherical shape was observed as the RH was increased to between 35 % at −10 °C and 80 % at −38 °C, confirming previous calculations of the viscosity-transition conditions. Consequently, α-pinene SOA particles exist in a viscous state over a wide range of ambient conditions, including the cirrus region of the free troposphere. This has implications for the physical, chemical, and ice-nucleation properties of SOA and SOA-coated particles in the atmosphere

Observation of viscosity transition in alpha-pinene secondary organic aerosol

Under certain conditions, secondary organic aerosol (SOA) particles can exist in the atmosphere in an amorphous solid or semi-solid state. To determine their relevance to processes such as ice nucleation or chemistry occurring within particles requires knowledge of the temperature and relative humidity (RH) range for SOA to exist in these states. In the Cosmics Leaving Outdoor Droplets (CLOUD) experiment at The European Organisation for Nuclear Research (CERN), we deployed a new in situ optical method to detect the viscous state of alpha-pinene SOA particles and measured their transition from the amorphous highly viscous state to states of lower viscosity. The method is based on the depolarising properties of laboratory-produced non-spherical SOA particles and their transformation to non-depolarising spherical particles at relative humidities near the deliquescence point. We found that particles formed and grown in the chamber developed an asymmetric shape through coagulation. A transition to a spherical shape was observed as the RH was increased to between 35aEuro-% at -10aEuro-A degrees C and 80aEuro-% at -38aEuro-A degrees C, confirming previous calculations of the viscosity-transition conditions. Consequently, alpha-pinene SOA particles exist in a viscous state over a wide range of ambient conditions, including the cirrus region of the free troposphere. This has implications for the physical, chemical, and ice-nucleation properties of SOA and SOA-coated particles in the atmosphere.Peer reviewe

Observation of viscosity transition in α-pinene secondary organic aerosol

Under certain conditions, secondary organic aerosol (SOA) particles can exist in the atmosphere in an amorphous solid or semi-solid state. To determine their relevance to processes such as ice nucleation or chemistry occurring within particles requires knowledge of the temperature and relative humidity (RH) range for SOA to exist in these states. In the Cosmics Leaving Outdoor Droplets (CLOUD) experiment at The European Organisation for Nuclear Research (CERN), we deployed a new in situ optical method to detect the viscous state of α-pinene SOA particles and measured their transition from the amorphous highly viscous state to states of lower viscosity. The method is based on the depolarising properties of laboratory-produced non-spherical SOA particles and their transformation to non-depolarising spherical particles at relative humidities near the deliquescence point. We found that particles formed and grown in the chamber developed an asymmetric shape through coagulation. A transition to a spherical shape was observed as the RH was increased to between 35 % at −10 °C and 80 % at −38 °C, confirming previous calculations of the viscosity-transition conditions. Consequently, α-pinene SOA particles exist in a viscous state over a wide range of ambient conditions, including the cirrus region of the free troposphere. This has implications for the physical, chemical, and ice-nucleation properties of SOA and SOA-coated particles in the atmosphere

The Cloud Particle Spectrometer with Polarization Detection (CPSPD): A next generation open-path cloud probe for distinguishing liquid cloud droplets from ice crystals

The differentiation of small water droplets and ice crystals by in situ measurements, in the size range < 50 μm, remains a challenge and the lack of such measurements is an obstacle to progress in understanding ice formation in clouds. A new microphysical instrument, the Cloud Particle Spectrometer with Polarization Detection (CPSPD), has been developed that measures light intensity scattered (in forward and backward directions) by individual cloud particles that pass through a focused laser beam and derives their size and thermodynamic phase (liquid or ice) in the optical diameter range from 2 to 50 μm. The optical equivalent diameter is derived from the light scattered in the forward direction. The change in polarization state of the incident light, caused by interaction with the cloud particle, is determined from the polarized components of the backscattered light. The CPSPD, along with several other cloud microphysical probes, has been flown on the University of North Dakota Citation aircraft in mixed phase clouds. It has also been deployed and operated at the Zugspitze research station studying mountain clouds. The preliminary results show that liquid cloud droplets can be distinguished from ice crystals and that the ice fraction can be estimated; an important parameter for better understanding of cloud processes, particularly that of glaciation

Development and characterization of an ice-selecting pumped counterflow virtual impactor (IS-PCVI) to study ice crystal residuals

Separation of particles that play a role in cloud activation and ice nucleation from interstitial aerosols has become necessary to further understand aerosol-cloud interactions. The pumped counterflow virtual impactor (PCVI), which uses a vacuum pump to accelerate the particles and increase their momentum, provides an accessible option for dynamic and inertial separation of cloud elements. However, the use of a traditional PCVI to extract large cloud hydrometeors is difficult mainly due to its small cut-size diameters ( 100 %), where a mixture of droplets and ice crystals was formed during the expansion experiment. In parallel, the flow conditions of the IS-PCVI were actively controlled, such that it separated ice crystals from a mixture of ice crystals and cloud droplets, which were of diameter  ≥  10 µm. These large ice crystals were passed through the heated evaporation section to remove the water content. Afterwards, the residuals were characterized with a suite of online and offline instruments downstream of the IS-PCVI. These results were used to assess the optimized operating parameters of the device in terms of (1) the critical cut-size diameter, (2) the transmission efficiency and (3) the counterflow-to-input flow ratio. Particle losses were characterized by comparing the residual number concentration to the rejected interstitial particle number concentration. Overall results suggest that the IS-PCVI enables inertial separation of particles with a volume-equivalent particle size in the range of  ~ 10–30 µm in diameter with small inadvertent intrusion (~  5 %) of unwanted particles