In situ characterization of mixed phase clouds using the Small Ice Detector and the Particle Phase Discriminator

Mixed phase clouds (MPCs) represent a great source of uncertainty for both climate predictions and weather forecasts. In particular, there is still a lack of understanding on how ice forms in these clouds. In this work we present a technique to analyze in situ measurements of MPCs performed with the latest instruments from the Small Ice Detector family. These instruments record high resolution scattering patterns of individual small cloud particles. For the analysis of the scattering patterns we developed an algorithm that can discriminate the phase of the cloud particles. In the case of a droplet, a Mie solution is fitted to the recorded pattern and the size of the corresponding particle is obtained, which allows for a size calibration of the instrument. In the case of an ice particle, its shape and roughness are deduced from the scattering pattern. We apply our data analysis method to measurements from three distinct MPC types. The results from laboratory measurements demonstrate that our technique can discriminate between droplets and ice particles in the same optical size range. This ability was verified by measurements at a mountain top station where we found an alternation of liquid and ice dominated cloud regions. The analysis of results from aircraft based measurements illustrates the ice detection threshold of the technique

In situ characterization of mixed phase clouds using the Small Ice Detector and the Particle Phase Discriminator

Mixed phase clouds (MPCs) represent a great source of uncertainty for both climate predictions and weather forecasts. In particular, there is still a lack of understanding on how ice forms in these clouds. In this work we present a technique to analyze in situ measurements of MPCs performed with the latest instruments from the Small Ice Detector family. These instruments record high-resolution scattering patterns of individual small cloud particles. For the analysis of the scattering patterns we developed an algorithm that can discriminate the phase of the cloud particles. In the case of a droplet, a Mie solution is fitted to the recorded pattern and the size of the corresponding particle is obtained, which allows for a size calibration of the instrument. In the case of an ice particle, its shape is deduced from the scattering pattern. We apply our data analysis method to measurements from three distinct MPC types. The results from laboratory measurements demonstrate that our technique can discriminate between droplets and ice particles in the same optical size range. This ability was verified by measurements at a mountain top station where we found an alternation of liquid- and ice-dominated cloud regions. The analysis of results from aircraft-based measurements illustrates the ice detection threshold of the technique

The Ice Selective Inlet: a novel technique for exclusive extraction of pristine ice crystals in mixed-phase clouds

Climate predictions are affected by high uncertainties partially due to an insufficient knowledge of aerosol-cloud interactions. One of the poorly understood processes is formation of mixed-phase clouds (MPCs) via heterogeneous ice nucleation. Field measurements of the atmospheric ice phase in MPCs are challenging due to the presence of supercooled liquid droplets. The Ice Selective Inlet (ISI), presented in this paper, is a novel inlet designed to selectively sample pristine ice crystals in mixed-phase clouds and extract the ice residual particles contained within the crystals for physical and chemical characterisation. Using a modular setup composed of a cyclone impactor, droplet evaporation unit and pumped counterflow virtual impactor (PCVI), the ISI segregates particles based on their inertia and phase, exclusively extracting small ice particles between 5 and 20 μm in diameter. The setup also includes optical particle spectrometers for analysis of the number size distribution and shape of the sampled hydrometeors. The novelty of the ISI is a droplet evaporation unit, which separates liquid droplets and ice crystals in the airborne state, thus avoiding physical impaction of the hydrometeors and limiting potential artifacts. The design and validation of the droplet evaporation unit is based on modelling studies of droplet evaporation rates and computational fluid dynamics simulations of gas and particle flows through the unit. Prior to deployment in the field, an inter-comparison of the WELAS optical particle size spectrometers and a characterisation of the transmission efficiency of the PCVI was conducted in the laboratory. The ISI was subsequently deployed during the Cloud and Aerosol Characterisation Experiment (CLACE) 2013 – an extensive international field campaign encompassing comprehensive measurements of cloud microphysics, as well as bulk aerosol, ice residual and ice nuclei properties. The campaign provided an important opportunity for a proof of concept of the inlet design. In this work we present the setup of the ISI, including the modelling and laboratory characterisation of its components, as well as a case study demonstrating the ISI performance in the field during CLACE 2013

Single-particle characterization of ice-nucleating particles and ice particle residuals sampled by three different techniques

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 February 2013 at the High Alpine Research Station Jungfraujoch (Switzerland). INPs and IPRs were analyzed offline by scanning electron microscopy and energy-dispersive X-ray microanalysis to determine their size, chemical composition and mixing state. Online analysis of the size and chemical composition of INP activated in FINCH was performed by laser ablation mass spectrometry. With all three INP/IPR separation techniques high abundances (median 20–70%) of instrumental contamination artifacts were observed (ISI: Si-O spheres, probably calibration aerosol; Ice-CVI: Al-O particles; FINCH + IN-PCVI: steel particles). After removal of the instrumental contamination particles, silicates, Ca-rich particles, carbonaceous material and metal oxides were the major INP/IPR particle types obtained by all three techniques. In addition, considerable amounts (median abundance mostly a few percent) of soluble material (e.g., sea salt, sulfates) were observed. As these soluble particles are often not expected to act as INP/IPR, we consider them as potential measurement artifacts. Minor types of INP/IPR include soot and Pb-bearing particles. The Pb-bearing particles are mainly present as an internal mixture with other particle types. Most samples showed a maximum of the INP/IPR size distribution at 200–400 nm in geometric diameter. In a few cases, a second supermicron maximum was identified. Soot/carbonaceous material and metal oxides were present mainly in the sub-micrometer range. Silicates and Ca-rich particles were mainly found with diameters above 1 μm (using ISI and FINCH), in contrast to the Ice-CVI which also sampled many submicron particles of both groups. Due to changing meteorological conditions, the INP/IPR composition was highly variable if different samples were compared. Thus, the observed discrepancies between the different separation techniques may partly result from the non-parallel sampling. The differences of the particle group relative number abundance as well as the mixing state of INP/IPR clearly demonstrate the need of further studies to better understand the influence of the separation techniques on the INP/IPR chemical composition. Also, it must be concluded that the abundance of contamination artifacts in the separated INP and IPR is generally large and should be corrected for, emphasizing the need for the accompanying chemical measurements. Thus, further work is needed to allow for routine operation of the three separation techniques investigated

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

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

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 CLOUD experiment at CERN, we deployed a new in-situ optical method to detect the viscosity of α-pinene SOA particles and measured their transition from the amorphous viscous to liquid state. The method is based on the depolarising properties of laboratory-produced non-spherical SOA particles and their transformation to non-depolarising spherical liquid particles during deliquescence. We found that particles formed and grown in the chamber developed an asymmetric shape through coagulation. A transition to 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

In situ characterization of mixed phase clouds using the Small Ice Detector and the Particle Phase Discriminator

Mixed phase clouds (MPCs) represent a great source of uncertainty for both climate predictions and weather forecasts. In particular, there is still a lack of understanding on how ice forms in these clouds. In this work we present a technique to analyze in situ measurements of MPCs performed with the latest instruments from the Small Ice Detector family. These instruments record high-resolution scattering patterns of individual small cloud particles. For the analysis of the scattering patterns we developed an algorithm that can discriminate the phase of the cloud particles. In the case of a droplet, a Mie solution is fitted to the recorded pattern and the size of the corresponding particle is obtained, which allows for a size calibration of the instrument. In the case of an ice particle, its shape is deduced from the scattering pattern. We apply our data analysis method to measurements from three distinct MPC types. The results from laboratory measurements demonstrate that our technique can discriminate between droplets and ice particles in the same optical size range. This ability was verified by measurements at a mountain top station where we found an alternation of liquid- and ice-dominated cloud regions. The analysis of results from aircraft-based measurements illustrates the ice detection threshold of the technique

The Ice Selective Inlet: A novel technique for exclusive extraction of pristine ice crystals in mixed-phase clouds

Climate predictions are affected by high uncertainties partially due to an insufficient knowledge of aerosol–cloud interactions. One of the poorly understood processes is formation of mixed-phase clouds (MPCs) via heterogeneous ice nucleation. Field measurements of the atmospheric ice phase in MPCs are challenging due to the presence of much more numerous liquid droplets. The Ice Selective Inlet (ISI), presented in this paper, is a novel inlet designed to selectively sample pristine ice crystals in mixed-phase clouds and extract the ice residual particles contained within the crystals for physical and chemical characterization. Using a modular setup composed of a cyclone impactor, droplet evaporation unit and pumped counterflow virtual impactor (PCVI), the ISI segregates particles based on their inertia and phase, exclusively extracting small ice particles between 5 and 20 μm in diameter. The setup also includes optical particle spectrometers for analysis of the number size distribution and shape of the sampled hydrometeors. The novelty of the ISI is a droplet evaporation unit, which separates liquid droplets and ice crystals in the airborne state, thus avoiding physical impaction of the hydrometeors and limiting potential artefacts. The design and validation of the droplet evaporation unit is based on modelling studies of droplet evaporation rates and computational fluid dynamics simulations of gas and particle flows through the unit. Prior to deployment in the field, an inter-comparison of the optical particle size spectrometers and a characterization of the transmission efficiency of the PCVI was conducted in the laboratory. The ISI was subsequently deployed during the Cloud and Aerosol Characterization Experiment (CLACE) 2013 and 2014 – two extensive international field campaigns encompassing comprehensive measurements of cloud microphysics, as well as bulk aerosol, ice residual and ice nuclei properties. The campaigns provided an important opportunity for a proof of concept of the inlet design. In this work we present the setup of the ISI, including the modelling and laboratory characterization of its components, as well as field measurements demonstrating the ISI performance and validating the working principle of the inlet. Finally, measurements of biological aerosol during a Saharan dust event (SDE) are presented, showing a first indication of enrichment of bio-material in sub-2 μm ice residuals

The Ice Selective Inlet: a novel technique for exclusive extraction of pristine ice crystals in mixed-phase clouds

Climate predictions are affected by high uncertainties partially due to an insufficient knowledge of aerosol–cloud interactions. One of the poorly understood processes is formation of mixed-phase clouds (MPCs) via heterogeneous ice nucleation. Field measurements of the atmospheric ice phase in MPCs are challenging due to the presence of much more numerous liquid droplets. The Ice Selective Inlet (ISI), presented in this paper, is a novel inlet designed to selectively sample pristine ice crystals in mixed-phase clouds and extract the ice residual particles contained within the crystals for physical and chemical characterization. Using a modular setup composed of a cyclone impactor, droplet evaporation unit and pumped counterflow virtual impactor (PCVI), the ISI segregates particles based on their inertia and phase, exclusively extracting small ice particles between 5 and 20 μm in diameter. The setup also includes optical particle spectrometers for analysis of the number size distribution and shape of the sampled hydrometeors. The novelty of the ISI is a droplet evaporation unit, which separates liquid droplets and ice crystals in the airborne state, thus avoiding physical impaction of the hydrometeors and limiting potential artefacts. The design and validation of the droplet evaporation unit is based on modelling studies of droplet evaporation rates and computational fluid dynamics simulations of gas and particle flows through the unit. Prior to deployment in the field, an inter-comparison of the optical particle size spectrometers and a characterization of the transmission efficiency of the PCVI was conducted in the laboratory. The ISI was subsequently deployed during the Cloud and Aerosol Characterization Experiment (CLACE) 2013 and 2014 – two extensive international field campaigns encompassing comprehensive measurements of cloud microphysics, as well as bulk aerosol, ice residual and ice nuclei properties. The campaigns provided an important opportunity for a proof of concept of the inlet design. In this work we present the setup of the ISI, including the modelling and laboratory characterization of its components, as well as field measurements demonstrating the ISI performance and validating the working principle of the inlet. Finally, measurements of biological aerosol during a Saharan dust event (SDE) are presented, showing a first indication of enrichment of bio-material in sub-2 μm ice residuals